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  • 1. Aartsen, M. G.
    et al.
    Ackermann, M.
    Adams, J.
    Aguilar, J. A.
    Ahlers, M.
    Ahrens, M.
    Altmann, D.
    Anderson, T.
    Arguelles, C.
    Arlen, T. C.
    Auffenberg, J.
    Bai, X.
    Barwick, S. W.
    Baum, V.
    Beatty, J. J.
    Tjus, J. Becker
    Becker, K. -H
    BenZvi, S.
    Berghaus, P.
    Berley, D.
    Bernardini, E.
    Bernhard, A.
    Besson, D. Z.
    Binder, G.
    Bindig, D.
    Bissok, M.
    Blaufuss, E.
    Blumenthal, J.
    Boersma, David J.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Fysiska sektionen, Institutionen för fysik och astronomi, Högenergifysik.
    Bohm, C.
    Bos, F.
    Bose, D.
    Boeser, S.
    Botner, Olga
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Fysiska sektionen, Institutionen för fysik och astronomi, Högenergifysik.
    Brayeur, L.
    Bretz, H. P.
    Brown, A. M.
    Casey, J.
    Casier, M.
    Cheung, E.
    Chirkin, D.
    Christov, A.
    Christy, B.
    Clark, K.
    Classen, L.
    Clevermann, F.
    Coenders, S.
    Cowen, D. F.
    Silva, A. H. Cruz
    Danninger, M.
    Daughhetee, J.
    Davis, J. C.
    Day, M.
    De Andre, J. P. A. M.
    DeClercq, C.
    De Ridder, S.
    Desiati, P.
    De Vries, K. D.
    Dewith, M.
    DeYoung, T.
    Diaz-Velez, J. C.
    Dunkman, M.
    Eagan, R.
    Eberhardt, B.
    Eichmann, B.
    Eisch, J.
    Euler, Sebastian
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Fysiska sektionen, Institutionen för fysik och astronomi, Högenergifysik.
    Evenson, P. A.
    Fadiran, O.
    Fazely, A. R.
    Fedynitch, A.
    Feintzeig, J.
    Felde, J.
    Feusels, T.
    Filimonov, K.
    Finley, C.
    Fischer-Wasels, T.
    Flis, S.
    Franckowiak, A.
    Frantzen, K.
    Fuchs, T.
    Gaisser, T. K.
    Gaior, R.
    Gallagher, J.
    Gerhardt, L.
    Gier, D.
    Gladstone, L.
    Glusenkamp, T.
    Goldschmidt, A.
    Golup, G.
    Gonzalez, J. G.
    Goodman, J. A.
    Gora, D.
    Grant, D.
    Gretskov, P.
    Groh, J. C.
    Gro, A.
    Ha, C.
    Haack, C.
    Ismail, A. Haj
    Hallen, P.
    Hallgren, Allan
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Fysiska sektionen, Institutionen för fysik och astronomi, Högenergifysik.
    Halzen, F.
    Hanson, K.
    Hebecker, D.
    Heereman, D.
    Heinen, D.
    Helbing, K.
    Hellauer, R.
    Hellwig, D.
    Hickford, S.
    Hill, G. C.
    Hoffman, K. D.
    Hoffmann, R.
    Homeier, A.
    Hoshina, K.
    Huang, F.
    Huelsnitz, W.
    Hulth, P. O.
    Hultqvist, K.
    Hussain, S.
    Ishihara, A.
    Jacobi, E.
    Jacobsen, J.
    Jagielski, K.
    Japaridze, G. S.
    Jero, K.
    Jlelati, O.
    Jurkovic, M.
    Kaminsky, B.
    Kappes, A.
    Karg, T.
    Karle, A.
    Kauer, M.
    Keivani, A.
    Kelley, J. L.
    Kheirandish, A.
    Kiryluk, J.
    Klaes, J.
    Klein, S. R.
    Koehne, J. H.
    Kohnen, G.
    Kolanoski, H.
    Koob, A.
    Koepke, L.
    Kopper, C.
    Kopper, S.
    Koskinen, D. J.
    Kowalski, M.
    Kriesten, A.
    Krings, K.
    Kroll, G.
    Kroll, M.
    Kunnen, J.
    Kurahashi, N.
    Kuwabara, T.
    Labare, M.
    Larsen, D. T.
    Larson, M. J.
    Lesiak-Bzdak, M.
    Leuermann, M.
    Leute, J.
    Luenemann, J.
    Madsen, J.
    Maggi, G.
    Maruyama, R.
    Mase, K.
    Matis, H. S.
    Maunu, R.
    McNally, F.
    Meagher, K.
    Medici, M.
    Meli, A.
    Meures, T.
    Miarecki, S.
    Middell, E.
    Middlemas, E.
    Milke, N.
    Miller, J.
    Mohrmann, L.
    Montaruli, T.
    Morse, R.
    Nahnhauer, R.
    Naumann, U.
    Niederhausen, H.
    Nowicki, S. C.
    Nygren, D. R.
    Obertacke, A.
    Odrowski, S.
    Olivas, A.
    Omairat, A.
    O'Murchadha, A.
    Palczewski, T.
    Paul, L.
    Penek, Oe.
    Pepper, J. A.
    Perez De Los Heros, Carlos
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Fysiska sektionen, Institutionen för fysik och astronomi, Högenergifysik.
    Pfendner, C.
    Pieloth, D.
    Pinat, E.
    Posselt, J.
    Price, P. B.
    Przybylski, G. T.
    Puetz, J.
    Quinnan, M.
    Raedel, L.
    Rameez, M.
    Rawlins, K.
    Redl, P.
    Rees, I.
    Reimann, R.
    Relich, M.
    Resconi, E.
    Rhode, W.
    Richman, M.
    Riedel, B.
    Robertson, S.
    Rodrigues, J. P.
    Rongen, M.
    Rott, C.
    Ruhe, T.
    Ruzybayev, B.
    Ryckbosch, D.
    Saba, S. M.
    Sander, H. -G
    Sandroos, J.
    Santander, M.
    Sarkar, S.
    Schatto, K.
    Scheriau, F.
    Schmidt, T.
    Schmitz, M.
    Schoenen, S.
    Schoeneberg, S.
    Schoenwald, A.
    Schukraft, A.
    Schulte, L.
    Schulz, O.
    Seckel, D.
    Sestayo, Y.
    Seunarine, S.
    Shanidze, R.
    Smith, M. W. E.
    Soldin, D.
    Spiczak, G. M.
    Spiering, C.
    Stamatikos, M.
    Stanev, T.
    Stanisha, N. A.
    Stasik, A.
    Stezelberger, T.
    Stokstad, R. G.
    Stoessl, A.
    Strahler, E. A.
    Ström, Rickard
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Fysiska sektionen, Institutionen för fysik och astronomi, Högenergifysik.
    Strotjohann, N. L.
    Sullivan, G. W.
    Taavola, Henric
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Fysiska sektionen, Institutionen för fysik och astronomi, Högenergifysik.
    Taboada, I.
    Tamburro, A.
    Tepe, A.
    Ter-Antonyan, S.
    Terliuk, A.
    Tesic, G.
    Tilav, S.
    Toale, P. A.
    Tobin, M. N.
    Tosi, D.
    Tselengidou, M.
    Unger, Eva
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Usner, M.
    Vallecorsa, S.
    Van Eijndhoven, N.
    Vandenbroucke, J.
    Van Santen, J.
    Vehring, M.
    Voge, M.
    Vraeghe, M.
    Walck, C.
    Wallraff, M.
    Weaver, Ch.
    Wellons, M.
    Wendt, C.
    Westerhoff, S.
    Whelan, B. J.
    Whitehorn, N.
    Wichary, C.
    Wiebe, K.
    Wiebusch, C. H.
    Williams, D. R.
    Wissing, H.
    Wolf, M.
    Wood, T. R.
    Woschnagg, K.
    Xu, D. L.
    Xu, X. W.
    Yanez, J. P.
    Yodh, G.
    Yoshida, S.
    Zarzhitsky, P.
    Ziemann, J.
    Zierke, S.
    Zoll, M.
    Morik, K.
    Development of a general analysis and unfolding scheme and its application to measure the energy spectrum of atmospheric neutrinos with IceCube2015Ingår i: European Physical Journal C, ISSN 1434-6044, E-ISSN 1434-6052, Vol. 75, nr 3, artikel-id 116Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    We present the development and application of a generic analysis scheme for the measurement of neutrino spectra with the IceCube detector. This scheme is based on regularized unfolding, preceded by an event selection which uses a Minimum Redundancy Maximum Relevance algorithm to select the relevant variables and a random forest for the classification of events. The analysis has been developed using IceCube data from the 59-string configuration of the detector. 27,771 neutrino candidates were detected in 346 days of livetime. A rejection of 99.9999 % of the atmospheric muon background is achieved. The energy spectrum of the atmospheric neutrino flux is obtained using the TRUEE unfolding program. The unfolded spectrum of atmospheric muon neutrinos covers an energy range from 100 GeV to 1 PeV. Compared to the previous measurement using the detector in the 40-string configuration, the analysis presented here, extends the upper end of the atmospheric neutrino spectrum by more than a factor of two, reaching an energy region that has not been previously accessed by spectral measurements.

  • 2.
    Abdelhamid, Hani Nasser
    et al.
    Stockholm Univ, Inorgan & Struct Chem, SE-10691 Stockholm, Sweden;Stockholm Univ, Berzelii Ctr EXSELENT Porous Mat, Dept Mat & Environm Chem, SE-10691 Stockholm, Sweden.
    Huang, Zhehao
    Stockholm Univ, Inorgan & Struct Chem, SE-10691 Stockholm, Sweden;Stockholm Univ, Berzelii Ctr EXSELENT Porous Mat, Dept Mat & Environm Chem, SE-10691 Stockholm, Sweden.
    El-Zohry, Ahmed
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Zheng, Haoquan
    Stockholm Univ, Inorgan & Struct Chem, SE-10691 Stockholm, Sweden;Stockholm Univ, Berzelii Ctr EXSELENT Porous Mat, Dept Mat & Environm Chem, SE-10691 Stockholm, Sweden.
    Zou, Xiaodong
    Stockholm Univ, Inorgan & Struct Chem, SE-10691 Stockholm, Sweden;Stockholm Univ, Berzelii Ctr EXSELENT Porous Mat, Dept Mat & Environm Chem, SE-10691 Stockholm, Sweden.
    A Fast and Scalable Approach for Synthesis of Hierarchical Porous Zeolitic Imidazolate Frameworks and One-Pot Encapsulation of Target Molecules2017Ingår i: Inorganic Chemistry, ISSN 0020-1669, E-ISSN 1520-510X, Vol. 56, nr 15, s. 9139-9146Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    A trimethylamine (TEA)-assisted synthesis approach that combines the preparation of hierarchical porous zeolitic, imidazolate framework ZIF-8, nanoparticles and one-pot encapsulation of target molecules is presented. Two dye molecules, rhodamine B (RhB) and methylene blue (MB), and one protein (bovine serum albumin, BSA) were, tested as the target molecules. The addition of TEA into the solution of zinc nitrate promoted the formation of ZnO nanocrystals, which rapidly transformed to ZIF-8 nanoparticles after the addition of the linker 2-methylimidazole (Hmim): Hierarchical porous dye@ZIF-8 nanoparticles with high crystallinity, large BET surface areas (1300-2500 m(2)/g), and large pore Volatiles (0.5-1.0 cm(3)/g) could be synthesized. The synthesis procedure was fast (down to 2 min) and scalable. The Hmim/Zn ratio could be greatly reduced (down to 2:1) compared to previously reported ones. The surface areas, and the mesopore size, structure, and density could be modified by changing the TEA or dye concentrations, or by postsynthetic treatment using reflux in methanol. This synthesis and one-pot encapsulation approach is simple and can be readily scaled Up. The photophysical properties such as lifetime and photostability of the dyes could be tuned via encapsulation. The lifetimes of the encapsulated dyes were increased by 3-27-fold for RhB@ZIF-8 and by 20-fold for MB@ZIF-8, compared to those of the corresponding free dyes. The synthesis approach is general, which was successfully applied for encapsulation of protein BSA. It could also be extended for the synthesis of hierarchical porous cobalt-based ZIP (dye@ZIF-67).

  • 3.
    Abdelhamid, Hani Nasser
    et al.
    Stockholm Univ, Dept Mat & Environm Chem, Berzelii Ctr EXSELENT Porous Mat, SE-10691 Stockholm, Sweden;Assiut Univ, Dept Chem, Assiut 71515, Egypt.
    Wilk-Kozubek, Magdalena
    Stockholm Univ, Dept Mat & Environm Chem, Berzelii Ctr EXSELENT Porous Mat, SE-10691 Stockholm, Sweden;PORT Polish Ctr Technol Dev, Dept Nanotechnol, 147 Stablowicka St, PL-54066 Wroclaw, Poland.
    El-Zohry, Ahmed
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Gomez, Antonio Bermejo
    Stockholm Univ, Dept Organ Chem, SE-10691 Stockholm, Sweden.
    Valiente, Alejandro
    Stockholm Univ, Dept Organ Chem, SE-10691 Stockholm, Sweden.
    Martin-Matute, Belen
    Stockholm Univ, Dept Organ Chem, SE-10691 Stockholm, Sweden.
    Mudring, Anja-Verena
    Stockholm Univ, Dept Mat & Environm Chem, Berzelii Ctr EXSELENT Porous Mat, SE-10691 Stockholm, Sweden.
    Zou, Xiaodong
    Stockholm Univ, Dept Mat & Environm Chem, Berzelii Ctr EXSELENT Porous Mat, SE-10691 Stockholm, Sweden.
    Luminescence properties of a family of lanthanide metal-organic frameworks2019Ingår i: Microporous and Mesoporous Materials, ISSN 1387-1811, E-ISSN 1873-3093, Vol. 279, s. 400-406Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Two isostructural series of lanthanide metal-organic frameworks denoted as SUMOF-7II (Ln) and SUMOF-7IIB (Ln) (Ln = La, Ce, Pr, Nd, Sm, Eu, and Gd) were synthesized using4,4',4 ''-(pyridine-2,4,6-triyl)tris(benzoic acid) (H(3)L2) and a mixture of H(3)L2 and 4,4',4 ''-(benzene-1,3,5-triyl)tris(benzoic acid) (H3BTB) as linkers, respectively. Both series were characterized using powder X-ray diffraction (PXRD), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), thermal analysis (TGA), and photoluminescence spectroscopy. Photoluminescence measurements show that Eu-MOFs demonstrate a red emission while Pr- and Nd-MOFs display an emission in the near-infrared (NIR) range. On the other hand, La-, Ce-, Sm- and Gd-MOFs exhibit only a ligand-centered emission. The average luminescence lifetimes in the SUMOF-7IIB series are 1.3-1.4-fold longer than the corresponding ones in the SUMOF-7II series. SUMOF-7IIs show a good photo- and thermal stability. Altogether, the properties of SUMOF-7II and SUMOF-7IIB render them promising materials for applications including sensing, biosensing, and telecommunications.

  • 4.
    Abdellah, Mohamed
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi. South Valley Univ, Qena Fac Sci, Dept Chem, Qena 83523, Egypt..
    El-Zohry, Ahmed M.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Antila, Liisa J.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Windle, Christopher D.
    Univ Cambridge, Dept Chem, Christian Doppler Lab Sustainable SynGas Chem, Lensfield Rd, Cambridge CB2 1EW, England..
    Reisner, Erwin
    Univ Cambridge, Dept Chem, Christian Doppler Lab Sustainable SynGas Chem, Lensfield Rd, Cambridge CB2 1EW, England..
    Hammarström, Leif
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Time-Resolved IR Spectroscopy Reveals a. Mechanism with TiO2 as a Reversible Electron Acceptor in a TiO2-Re Catalyst System for CO2 Photoreduction2017Ingår i: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 139, nr 3, s. 1226-1232Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Attaching the phosphonated molecular catalyst [(ReBr)-Br-I(bpy)-(CO)(3)](0) to the wide-bandgap semiconductor TiO2 strongly enhances the rate of visible-light-driven reduction of CO2 to CO in dimethylformamide with triethanolamine (TEOA) as sacrificial electron donor. Herein, we show by transient mid-IR spectroscopy that the mechanism of catalyst photoreduction is initiated by ultrafast electron injection into TiO2, followed by rapid (ps-ns) and sequential two-electron oxidation of TEOA that is coordinated to the Re center. The injected electrons can be stored in the conduction band of TiO2 on an ms-s time scale, and we propose that they lead to further reduction of the Re catalyst and completion of the catalytic cycle. Thus, the excited Re catalyst gives away one electron and would eventually get three electrons back. The function of an electron reservoir would represent a role for TiO2 in photocatalytic CO2 reduction that has previously not been considered. We propose that the increase in photocatalytic activity upon heterogenization of the catalyst to TiO2 is due to the slow charge recombination and the high oxidative power of the Re-II species after electron injection as compared to the excited MLCT state of the unbound Re catalyst or when immobilized on ZrO2, which results in a more efficient reaction with TEOA.

  • 5.
    Abdellah, Mohamed
    et al.
    Lund Univ, Div Chem Phys, Box 124, S-22100 Lund, Sweden.;Lund Univ, NanoLund, Box 124, S-22100 Lund, Sweden.;South Valley Univ, Qena Fac Sci, Dept Chem, Qena 83523, Egypt..
    Poulsen, Felipe
    Univ Copenhagen, Dept Chem, DK-2100 Copenhagen, Denmark..
    Zhu, Qiushi
    Lund Univ, Div Chem Phys, Box 124, S-22100 Lund, Sweden.;Lund Univ, NanoLund, Box 124, S-22100 Lund, Sweden..
    Zhu, Nan
    Tech Univ Denmark, Dept Chem, Kemitorvet Bldg 207, DK-2800 Lyngby, Denmark.;Dalian Univ Technol, Zhang Dayu Sch Chem, Dalian 116024, Peoples R China..
    Zidek, Karel
    Acad Sci Czech Republ, Inst Plasma Phys, Reg Ctr Special Opt & Optoelect Syst TOPTEC, Za Slovankou 1782-3, Prague 18200 8, Czech Republic..
    Chabera, Pavel
    Lund Univ, Div Chem Phys, Box 124, S-22100 Lund, Sweden.;Lund Univ, NanoLund, Box 124, S-22100 Lund, Sweden..
    Corti, Annamaria
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Hansen, Thorsten
    Univ Copenhagen, Dept Chem, DK-2100 Copenhagen, Denmark..
    Chi, Qijin
    Tech Univ Denmark, Dept Chem, Kemitorvet Bldg 207, DK-2800 Lyngby, Denmark..
    Canton, Sophie E.
    DESY, Attosecond Sci Grp, Notkestr 85, D-22607 Hamburg, Germany.;ELI HU Nonprofit Ltd, ELI ALPS, Dugonics Ter 13, H-6720 Szeged, Hungary..
    Zheng, Kaibo
    Lund Univ, Div Chem Phys, Box 124, S-22100 Lund, Sweden.;Lund Univ, NanoLund, Box 124, S-22100 Lund, Sweden.;Qatar Univ, Coll Engn, Gas Proc Ctr, POB 2713, Doha, Qatar..
    Pullerits, Tonu
    Lund Univ, Div Chem Phys, Box 124, S-22100 Lund, Sweden.;Lund Univ, NanoLund, Box 124, S-22100 Lund, Sweden..
    Drastic difference between hole and electron injection through the gradient shell of CdxSeyZn1−xS1−y quantum dots2017Ingår i: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 9, nr 34, s. 12503-12508Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Ultrafast fluorescence spectroscopy was used to investigate the hole injection in CdxSeyZn1-xS1-y gradient core-shell quantum dot (CSQD) sensitized p-type NiO photocathodes. A series of CSQDs with a wide range of shell thicknesses was studied. Complementary photoelectrochemical cell measurements were carried out to confirm that the hole injection from the active core through the gradient shell to NiO takes place. The hole injection from the valence band of the QDs to NiO depends much less on the shell thickness when compared to the corresponding electron injection to n-type semiconductor (ZnO). We simulate the charge carrier tunneling through the potential barrier due to the gradient shell by numerically solving the Schrodinger equation. The details of the band alignment determining the potential barrier are obtained from X-ray spectroscopy measurements. The observed drastic differences between the hole and electron injection are consistent with a model where the hole effective mass decreases, while the gradient shell thickness increases.

  • 6.
    Abdellah, Mohamed
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi. South Valley Univ, Qena Fac Sci, Dept Chem, Qena 83523, Egypt.
    Zhang, Shihuai
    Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Wang, Mei
    Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China..
    Hammarström, Leif
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Competitive Hole Transfer from CdSe Quantum Dots to Thiol Ligands in CdSe-Cobaloxime Sensitized NiO Films Used as Photocathodes for H-2 Evolution2017Ingår i: ACS Energy Letters, ISSN 2380-8195, Vol. 2, nr 11, s. 2576-2580Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Quantum dot (QD) sensitized NiO photocathodes rely on efficient photoinduced hole injection into the NiO valence band. A system of a mesoporous NiO film co-sensitized with CdSe QDs and a molecular proton reduction catalyst was studied. While successful electron transfer from the excited QDs to the catalyst is observed, most of the photogenerated holes are instead quenched very rapidly (ps) by hole trapping at the surface thiols of the capping agent used as linker molecules. We confirmed our conclusion by first using a thiol free capping agent and second varying the thiol concentration on the QD's surface. The later resulted in faster hole trapping as the thiol concentration increased. We suggest that this hole trapping by the linker limits the H-2 yield for this photocathode in a device.

  • 7.
    Abdi-Jalebi, Mojtaba
    et al.
    Univ Cambridge, Dept Phys, Cavendish Lab, JJ Thomson Ave, Cambridge, England.
    Pazoki, Meysam
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Tekniska sektionen, Institutionen för teknikvetenskaper, Fasta tillståndets fysik.
    Philippe, Bertrand
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Fysiska sektionen, Institutionen för fysik och astronomi, Molekyl- och kondenserade materiens fysik.
    Dar, M. Ibrahim
    Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Lab Photon & Interfaces, Lausanne, Switzerland.
    Alsari, Mejd
    Univ Cambridge, Dept Phys, Cavendish Lab, JJ Thomson Ave, Cambridge, England.
    Sadhanala, Aditya
    Univ Cambridge, Dept Phys, Cavendish Lab, JJ Thomson Ave, Cambridge, England.
    Diyitini, Giorgio
    Univ Cambridge, Dept Mat Sci & Met, Charles Babbage Rd, Cambridge, England.
    Imani, Roghayeh
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Lilliu, Samuele
    Univ Sheffield, Dept Phys & Astron, Sheffield, S Yorkshire, England; UAE Ctr Crystallog, Dubai, U Arab Emirates.
    Kullgren, Jolla
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Rensmo, Håkan
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Fysiska sektionen, Institutionen för fysik och astronomi, Molekyl- och kondenserade materiens fysik.
    Gratzel, Michael
    Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Lab Photon & Interfaces, Lausanne, Switzerland.
    Friend, Richard H.
    Univ Cambridge, Dept Phys, Cavendish Lab, JJ Thomson Ave, Cambridge, England.
    Dedoping of Lead Halide Perovskites Incorporating Monovalent Cations2018Ingår i: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 12, nr 7, s. 7301-7311Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    We report significant improvements in the optoelectronic properties of lead halide perovskites with the addition of monovalent ions with ionic radii close to Pb2+. We investigate the chemical distribution and electronic structure of solution processed CH3NH3PbI3 perovskite structures containing Na+, Cu+, and Ag+, which are lower valence metal ions than Pb2+ but have similar ionic radii. Synchrotron X-ray diffraction reveals a pronounced shift in the main perovskite peaks for the monovalent cation-based films, suggesting incorporation of these cations into the perovskite lattice as well as a preferential crystal growth in Ag+ containing perovskite structures. Furthermore, the synchrotron X-ray photoelectron measurements show a significant change in the valence band position for Cu- and Ag-doped films, although the perovskite bandgap remains the same, indicating a shift in the Fermi level position toward the middle of the bandgap. Such a shift infers that incorporation of these monovalent cations dedope the n-type perovskite films when formed without added cations. This dedoping effect leads to cleaner bandgaps as reflected by the lower energetic disorder in the monovalent cation-doped perovskite thin films as compared to pristine films. We also find that in contrast to Ag+ and Cu+, Na+ locates mainly at the grain boundaries and surfaces. Our theoretical calculations confirm the observed shifts in X-ray diffraction peaks and Fermi level as well as absence of intrabandgap states upon energetically favorable doping of perovskite lattice by the monovalent cations. We also model a significant change in the local structure, chemical bonding of metal-halide, and the electronic structure in the doped perovskites. In summary, our work highlights the local chemistry and influence of monovalent cation dopants on crystallization and the electronic structure in the doped perovskite thin films.

  • 8.
    Abrahamsson, Maria
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström.
    Becker, Hans-Christian
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström.
    Hammarström, Leif
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Microsecond (MLCT)-M-3 excited state lifetimes in bis-tridentate Ru(II)-complexes: significant reductions of non-radiative rate constants2017Ingår i: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 46, nr 39, s. 13314-13321Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    In this paper we report the photophysical properties of a series of bis-tridentate Ru-II-complexes, based on the dqp-ligand (dqp = 2,6-di(quinolin-8-yl) pyridine), which display several microsecond long excited state lifetimes for triplet metal-to-ligand charge transfer ((MLCT)-M-3) at room temperature. Temperature dependence of the excited state lifetimes for [Ru(dqp)(2)](2+) and [Ru(dqp)(ttpy)](2+) (ttpy = 4'-tolyl-2,2': 6', 2 ''-terpyridine) is reported and radiative and non-radiative rate constants for the whole series are reported and discussed. We can confirm previous assumptions that the near-octahedricity of the bis-dqp complexes dramatically slows down activated decay at room temperature, as compared to most other and less long-lived bis-tridentate RuII-complexes, such as [Ru(tpy)(2)](2+) with tau = 0.25 ns at room temperature (tpy = 2,2': 6', 2 ''-terpyridine). Moreover, the direct non-radiative decay to the ground state is comparatively slow for similar to 700 nm room-temperature emission when considering the energy-gap law. Analysis of the 77 K emission spectra suggests that this effect is not primarily due to smaller excited state distortion than that for comparable complexes. Instead, an analysis of the photophysical parameters suggests a weaker singlet-triplet mixing in the MLCT state, which slows down both radiative and non-radiative decay.

  • 9. Achari, Muthuraaman Bhagavathi
    et al.
    Elumalai, Viswanathan
    Vlachopoulos, Nikolaos
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Safdari, Majid
    Gao, Jiajia
    Gardner, James M.
    Kloo, Lars
    A quasi-liquid polymer-based cobalt redox mediator electrolyte for dye-sensitized solar cells2013Ingår i: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 15, nr 40, s. 17419-17425Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Recently, cobalt redox electrolyte mediators have emerged as a promising alternative to the commonly used iodide/triiodide redox shuttle in dye-sensitized solar cells (DSCs). Here, we report the successful use of a new quasi-liquid, polymer-based electrolyte containing the Co3+/Co2+ redox mediator in 3-methoxy propionitrile solvent in order to overcome the limitations of high cell resistance, low diffusion coefficient and rapid recombination losses. The performance of the solar cells containing the polymer based electrolytes increased by a factor of 1.2 with respect to an analogous electrolyte without the polymer. The performances of the fabricated DSCs have been investigated in detail by photovoltaic, transient electron measurements, EIS, Raman and UV-vis spectroscopy. This approach offers an effective way to make high-performance and long-lasting DSCs.

  • 10.
    Adamovic, Nadja
    et al.
    TU Wien, ISAS, Vienna, Austria..
    Asinari, Pietro
    Politecn Torino, Dept Energy, Turin, Italy..
    Goldbeck, Gerhard
    Goldbeck Consulting Ltd, St Johns Innovat Ctr, Cambridge, England..
    Hashibon, Adham
    Fraunhofer Inst Mech Mat IWM, Freiburg, Germany..
    Hermansson, Kersti
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Hristova-Bogaerds, Denka
    DPI, Eindhoven, Netherlands..
    Koopmans, Rudolf
    Koopmans Consulting GmbH, Zurich, Switzerland..
    Verbrugge, Tom
    Dow Benelux BV, Hoek, Netherlands..
    Wimmer, Erich
    Mat Design, Le Mans, France..
    European Materials Modelling Council2017Ingår i: Proceedings Of The 4Th World Congress On Integrated Computational Materials Engineering (Icme 2017) / [ed] Mason, P Fisher, CR Glamm, R Manuel, MV Schmitz, GJ Singh, AK Strachan, A, Springer Publishing Company, 2017, s. 79-92Konferensbidrag (Refereegranskat)
    Abstract [en]

    The aim of the European Materials Modelling Council (EMMC) is to establish current and forward looking complementary activities necessary to bring the field of materials modelling closer to the demands of manufacturers (both small and large enterprises) in Europe. The ultimate goal is that materials modelling and simulation will become an integral part of product life cycle management in European industry, thereby making a strong contribution to enhance innovation and competitiveness on a global level. Based on intensive efforts in the past two years within the EMMC, which included numerous consultation and networking actions with representatives of all stakeholders including Modellers, Software Owners, Translators and Manufacturers in Europe, the EMMC identified and proposed a set of underpinning and enabling actions to increase the industrial exploitation of materials modelling in Europe. EMMC will pursue the following overarching objectives in order to bridge the gap between academic innovation and industrial application: enhance the interaction and collaboration between all stakeholders engaged in different types of materials modelling, including modellers, software owners, translators and manufacturers, facilitate integrated materials modelling in Europe building on strong and coherent foundations, coordinate and support actors and mechanisms that enable rapid transfer of materials modelling from academic innovation to the end users and potential beneficiaries in industry, achieve greater awareness and uptake of materials modelling in industry, in particular SMEs, elaborate Roadmaps that (i) identify major obstacles to widening the use of materials modelling and (ii) elaborate strategies to overcome them.

  • 11. Adamska-Venkatesh, Agnieszka
    et al.
    Mirmohades, Mohammad
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Sommer, Constanze
    Reijerse, Edward
    Lubitz, Wolfgang
    Lomoth, Reiner
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Hammarström, Leif
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Following [FeFe] Hydrogenase Active Site Intermediates by Flash Photolysis/Mid-IR ProbingManuskript (preprint) (Övrigt vetenskapligt)
  • 12.
    Agervald, Åsa
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Molekylär biomimetik. Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för fotokemi och molekylärvetenskap, Mikrobiell kemi.
    Camsund, Daniel
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Molekylär biomimetik.
    Stensjö, Karin
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Molekylär biomimetik.
    Lindblad, Peter
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Molekylär biomimetik.
    CRISPR in the extended hyp-operon of the cyanobacterium Nostoc sp. strain PCC 7120, characteristics and putative function(s)2012Ingår i: International journal of hydrogen energy, ISSN 0360-3199, E-ISSN 1879-3487, Vol. 37, nr 10, s. 8828-8833Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    The presence of small RNAs (sRNA) and their functions in transcriptional regulation has lately turned into a hot topic. Since cyanobacteria often face changes in the surrounding environment, they need to have a well working system for stress response. Quick adaption is necessary, and an RNA-based regulatory system is thus useful. One example of these sRNAs is CRISPRs. In this work we report the existence of a CRISPR within the hyp-operon (hyp genes encode proteins responsible for the maturation of hydrogenases) of the filamentous cyanobacterium Nostoc sp. strain PCC 7120. We present data concerning its characteristics and putative function(s) and raise the question concerning the importance of this CRISPR array and other CRISPR systems in general. In addition, we discuss the use of the CRISPR system as a potential bacterial genetic defence mechanism to achieve robust, cyanobacterial cultures in large scale, commercial production units.

  • 13.
    Aguirre Castillo, José
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Oorganisk kemi.
    Optimisation of the bottom stirring praxis in a LD-LBE converter: Investigations and tests on phosphorous removal, nitrogen as stirring gas, and slopping2015Självständigt arbete på avancerad nivå (yrkesexamen), 20 poäng / 30 hpStudentuppsats (Examensarbete)
    Abstract [sv]

    En järnmalmsbaserad stålproduktion börjar med att järnmalm matas i en masugn tillsammans med koks, kalk och tillsatsämnen. Ut kommer råjärn med höga kol och svavelhalter. Råjärnet transporteras till stålverket i så kallade torpedvagnar. I vissa stålverk, t.ex. SSAB Special Steels i Oxelösund, renas råjärnet från svavel i torpedvagnen. I andra stålverk svavelrenar man i separata skänkar. Svavelreningen sker med bland annat kalciumkarbid som binder till svavlet.

    Det svavelfattiga råjärnet måste sedan renas från kol för att bli stål. Det görs i en LD-konvertern (Linz Donawitz). LD-konvertern laddas med flytande råjärn som har en kolhalt på 4,5 procent och som är runt 1350 grader varmt. Råjärnet kyls genom att cirka 20 procent skrot tillsätts. En syrgaslans sänks sedan in i konvertern ovanför smältan och reningen startar.  Syrgaslansen blåser syrgas i ultraljudsfart vilket oxiderar en del av järnet, så väl som kol, kisel, mangan, fosfor and andra föroreningsämnen i råjärnet. Kol försvinner ur konvertern i form av kolmonoxidgas. Andra oxiderade föroreningar och järnoxid bildar tillsammans en så kallad slagg som flyter ovanpå smältan. Det tillsätts även så kallade slaggbildare som förbättrar upptaget av föroreningar i slaggen. Processen varar i cirka 17 minuter och är mycket beroende av slaggen som bildas. Kol försvinner ur konvertern i form av kolmonoxidgas. Under processens gång rör man om smältan med hjälp av gaser som spolas genom botten av konvertern. Omröringen jämnar ut smältans sammansättning och temperatur. När man inte länge behöver avlägsna kol stoppas processen. Stålets temperatur är då cirka 1700 grader och kolhalten ligger nära 0,05 procent.

    Stålet överförs sedan till en skänk för att skilja det ur slaggen. Stålet förädlas vidare i olika processer där sammansättningen justeras så att det möter kundens krav. Sedan gjuts stålet i strängar för transport till valsverk eller kunder.

    Denna studie behandlar bottenomrörningen under LD-processen i SSAB Special Steels's stålverk i Oxelösund. Omrörningen sker genom åtta porösa stenar i botten av konvertern som blåser med argon eller kväve. Gasflödet genom stenarna justeras genom ett ventilsystem. Under blåsningen rör man om med hjälp av förinställda program. Omrörningens primära funktion är att avlasta syrgaslansen. I fallen där ingen bottenomrörning finns måste syrgaslansen blåsa ”hårdare” på stålet för att avlägsna kol. Avlastningen som bottenomrörningen bidrar med gör att processen även kallas för LD-LBE, där LBE står för Lans Bubbling Equilibrium.

    Bottenomrörningen tros ha en positiv effekt på stålets rening från fosfor. Sedan tidigare vet man att temperatur och slaggsammansättning är de största faktorerna som påverkar fosforreningen. Fosfor tas lättare upp i slaggen vid låga temperaturen samt i slagg med högre kalkhalter. Olika omrörningsprogram testades och en bättre fosforrening nåddes. Bottenomrörningen visade sig ha positiva effekter som är teoretisk kopplade till kalksmältning. Två möjliga förklaringsmekanismer hittades.

    Studien undersökte även användningen av kväve som omrörningsgas istället för argon, då kväve är ekonomisk fördelaktig gentemot argon. Kväve finns inlöst i råjärnet som sätts in i konvertern. Kvävgasen försvinner ur stålet under och med hjälp av kolreningen. Det visade sig vara säkert att använda kväve från start fram till halva syrgasblåset på kvävekänsliga stålsorter, var efter man sedan byte till argon. Kväve som används sent under blåset visade ge högre kvävehalter.

    Urkok är en kraftig volymökning av slaggen som sker när bildad gas från reningen av smältan fångas i slaggen och får slaggen att ”koka över”. Urkok resulterar i ekonomiska förluster då slaggen som lämnar konvertern vid urkok är rik på järn. Bottenomrörningens eventuella påverkan på urkok studerades. Det visade sig att urkok inte kan undvikas genom att enbart optimera bottenomrörningen.

  • 14.
    Ahlberg, Patrik
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Tekniska sektionen, Institutionen för teknikvetenskaper, Fasta tillståndets elektronik.
    Johansson, Fredrik
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Fysiska sektionen, Institutionen för fysik och astronomi.
    Zhang, Zhibin
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Tekniska sektionen, Institutionen för teknikvetenskaper, Fasta tillståndets elektronik.
    Jansson, Ulf
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Oorganisk kemi.
    Zhang, Shi-Li
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Tekniska sektionen, Institutionen för teknikvetenskaper, Fasta tillståndets elektronik.
    Lindblad, Andreas
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Fysiska sektionen, Institutionen för fysik och astronomi.
    Nyberg, Tomas
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Tekniska sektionen, Institutionen för teknikvetenskaper, Fasta tillståndets elektronik.
    Defect formation in graphene during low-energy ion bombardment2016Ingår i: APL Materials, ISSN 2166-532X, Vol. 4, nr 4, artikel-id 046104Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    This letter reports on a systematic investigation of sputter induced damage in graphene caused by low energy Ar+ ion bombardment. The integral numbers of ions per area (dose) as well as their energies are varied in the range of a few eV's up to 200 eV. The defects in the graphene are correlated to the dose/energy and different mechanisms for the defect formation are presented. The energetic bombardment associated with the conventional sputter deposition process is typically in the investigated energy range. However, during sputter deposition on graphene, the energetic particle bombardment potentially disrupts the crystallinity and consequently deteriorates its properties. One purpose with the present study is therefore to demonstrate the limits and possibilities with sputter deposition of thin films on graphene and to identify energy levels necessary to obtain defect free graphene during the sputter deposition process. Another purpose is to disclose the fundamental mechanisms responsible for defect formation in graphene for the studied energy range.

  • 15.
    Ahlberg, Patrik
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Tekniska sektionen, Institutionen för teknikvetenskaper, Fasta tillståndets elektronik.
    Nyberg, Tomas
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Tekniska sektionen, Institutionen för teknikvetenskaper, Fasta tillståndets elektronik.
    Zhang, Shi-Li
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Tekniska sektionen, Institutionen för teknikvetenskaper, Fasta tillståndets elektronik.
    Zhang, Zhi-Bin
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Tekniska sektionen, Institutionen för teknikvetenskaper, Fasta tillståndets elektronik.
    Jansson, Ulf
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Oorganisk kemi.
    Toward synthesis of oxide films on graphene with sputtering based processes2016Ingår i: Journal of Vacuum Science & Technology B, ISSN 1071-1023, E-ISSN 1520-8567, Vol. 34, nr 4, artikel-id 040605Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    The impact of energetic particles associated with a sputter deposition process may introduce damage to single layer graphene films, making it challenging to apply this method when processing graphene. The challenge is even greater when oxygen is incorporated into the sputtering process as graphene can be readily oxidized. This work demonstrates a method of synthesizing ZnSn oxide on graphene without introducing an appreciable amount of defects into the underlying graphene. Moreover, the method is general and applicable to other oxides. The formation of ZnSn oxide is realized by sputter deposition of ZnSn followed by a postoxidation step. In order to prevent the underlying graphene from damage during the initial sputter deposition process, the substrate temperature is kept close to room temperature, and the processing pressure is kept high enough to effectively suppress energetic bombardment. Further, in the subsequent postannealing step, it is important not to exceed temperatures resulting in oxidation of the graphene. The authors conclude that postoxidation of ZnSn is satisfactorily performed at 300 degrees C in pure oxygen at reduced pressure. This process results in an oxidized ZnSn film while retaining the initial quality of the graphene film.

  • 16.
    Ahlstrand, Emma
    et al.
    Linnus Univ, Dept Chem & Biomed Sci, S-39182 Kalmar, Sweden.;Linnus Univ, Ctr Biomat Chem, S-39182 Kalmar, Sweden..
    Hermansson, Kersti
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Friedman, Ran
    Linnus Univ, Dept Chem & Biomed Sci, S-39182 Kalmar, Sweden.;Linnus Univ, Ctr Biomat Chem, S-39182 Kalmar, Sweden..
    Interaction Energies in Complexes of Zn and Amino Acids: A Comparison of Ab Initio and Force Field Based Calculations2017Ingår i: Journal of Physical Chemistry A, ISSN 1089-5639, E-ISSN 1520-5215, Vol. 121, nr 13, s. 2643-2654Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Zinc plays important roles in structural stabilization of proteins, eniyine catalysis, and signal transduction. Many Zn binding sites are located at the interface between the protein and the cellular fluid. In aqueous solutions, Zn ions adopt an octahedral coordination, while in proteins zinc can have different coordinations, with a tetrahedral conformation found most frequently. The dynainics of Zn binding to proteins and the formation of complexes that involve Zn are dictated by interactions between Zn and its binding partners. We calculated the interaction energies between Zn and its ligands in complexes that mimic protein binding sites and in Zn complexes of water and one or two amino acid moieties, using quantum mechanics (QM) and molecular mechanics (MM). It was found that MM calculations that neglect or only approximate polarizability did not reproduce even the relative order of the QM interaction energies in these complexes. Interaction energies calculated with the CHARMM-Diode polarizable force field agreed better with the ab initio results,:although the deviations between QM and MM were still rather large (40-96 kcallmol). In order to gain further insight into Zn ligand interactions, the free energies of interaction were estimated by QM calculations with continuum solvent representation, and we performed energy decomposition analysis calculations to examine the characteristics of the different complexes. The ligand-types were found to have high impact on the relative strength of polarization and electrostatic interactions. Interestingly, ligand ligand interactions did not play a significant role in the binding of Zn. Finally) analysis of ligand exchange energies suggests that carboxylates could be exchanged with water molecules, which explains the flexibility in Zn:binding dynamics. An exchange between earboxylate (Asp/Glii) and imidazole (His) is less likely.

  • 17.
    Ahlstrand, Emma
    et al.
    Linnæus University Centre for Biomaterials Chemistry.
    Spångberg, Daniel
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Hermansson, Kersti
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Friedman, Ran
    Interaction Energies Between Metal Ions (Zn2+ and Cd2+) and Biologically Relevant Ligands2013Ingår i: International Journal of Quantum Chemistry, ISSN 0020-7608, E-ISSN 1097-461X, Vol. 113, nr 23, s. 2554-2562Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Interactions between the group XII metals Zn2+ and Cd2+ and amino acid residues play an important role in biology due to the prevalence of the first and the toxicity of the second. Estimates of the interaction energies between the ions and relevant residues in proteins are however difficult to obtain. This study reports on calculated interaction energy curves for small complexes of Zn2+ or Cd2+ and amino acid mimics (acetate, methanethiolate, and imidazole) or water. Given that many applications and models (e.g., force fields, solvation models, etc.) begin with and rely on an accurate description of gas-phase interaction energies, this is where our focus lies in this study. Four density functional theory (DFT)-functionals and MP2 were used to calculate the interaction energies not only at the respective equilibrium distances but also at a relevant range of ion–ligand separation distances. The calculated values were compared with those obtained by CCSD(T). All DFT-methods are found to overestimate the magnitude of the interaction energy compared to the CCSD(T) reference values. The deviation was analyzed in terms of energy components from localized molecular orbital energy decomposition analysis scheme and is mostly attributed to overestimation of the polarization energy. MP2 shows good agreement with CCSD(T) [root mean square error (RMSE) = 1.2 kcal/mol] for the eight studied complexes at equilibrium distance. Dispersion energy differences at longer separation give rise to increased deviations between MP2 and CCSD(T) (RMSE = 6.4 kcal/mol at 3.0 Å). Overall, the results call for caution in applying DFT methods to metalloprotein model complexes even with closed-shell metal ions such as Zn2+ and Cd2+, in particular at ion–ligand separations that are longer than the equilibrium distances.

  • 18.
    Ahmadova, Nigar
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Molekylär biomimetik.
    Studies of the two redox active tyrosines in Photosystem II2017Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
    Abstract [en]

    Photosystem II is a unique enzyme which catalyzes light induced water oxidation. This process is driven by highly oxidizing ensemble of four Chl molecules, PD1, PD2, ChlD1 and ChlD2 called, P680. Excitation of one of the Chls in P680 leads to the primary charge separation, P680+Pheo-. Pheo- transfers electrons sequentially to the primary quinone acceptor QA and the secondary quinone acceptor QB. P680+ in turn extracts electrons from Mn4CaO5 cluster, a site for the water oxidation. There are two redox active tyrosines, TyrZ and TyrD, found in PSII. They are symmetrically located on the D1 and D2 central proteins. Only TyrZ acts as intermediate electron carrier between P680 and Mn4CaO5 cluster, while TyrD does not participate in the linear electron flow and stays oxidized under light conditions. Both tyrosines are involved in PCET.

    The reduced TyrD undergoes biphasic oxidation with the fast (msec-sec time range) and the slow (tens of seconds time range) kinetic phases. We assign these phases to two populations of PSII centers with proximal or distal water positions. We also suggest that the TyrD oxidation and stability is regulated by the new small lumenal protein subunit, PsbTn. The possible involvement of PsbTn protein in the proton translocation mechanism from TyrD is suggested.

    To assess the possible localization of primary cation in P680 the formation of the triplet state of P680 and the oxidation of TyrZ and TyrD were followed under visible and far-red light. We proposed that far-red light induces the cation formation on ChlD1.

    Transmembrane interaction between QB and TyrZ has been studied. The different oxidation yield of TyrZ, measured as a S1 split EPR signal was correlated to the conformational change of protein induced by the QB presence at the QB-site. The change is transferred via H-bonds to the corresponding His-residues via helix D of the D1 protein.

    Delarbeten
    1. The protonation state around Tyr(D)/Tyr((D)) over dot in photosystem II is reflected in its biphasic oxidation kinetics
    Öppna denna publikation i ny flik eller fönster >>The protonation state around Tyr(D)/Tyr((D)) over dot in photosystem II is reflected in its biphasic oxidation kinetics
    Visa övriga...
    2017 (Engelska)Ingår i: Biochimica et Biophysica Acta - Bioenergetics, ISSN 0005-2728, E-ISSN 1879-2650, Vol. 1858, nr 2, s. 147-155Artikel i tidskrift (Refereegranskat) Published
    Abstract [en]

    The tyrosine residue D2-Tyr160 (Tyr(D)) in photosystem II (PSII) can be oxidized through charge equilibrium with the oxygen evolving complex in PSII. The kinetics of the electron transfer from Tyr(D) has been followed using time resolved EPR spectroscopy after triggering the oxidation of pre-reduced Tyr(D) by a short laser flash. After its oxidation Tyro is observed as a neutral radical (Tyr((D)) over dot) indicating that the oxidation is coupled to a deprotonation event. The redox state of Tyro was reported to be determined by the two water positions identified in the crystal structure of PSII [Saito et al. (2013) Proc. Natl. Acad. Sci. USA 110, 7690]. To assess the mechanism of the proton coupled electron transfer of Tyr(D) the oxidation kinetics has been followed in the presence of deuterated buffers, thereby resolving the kinetic isotope effect (KIE) of Tyro oxidation at different H/D concentrations. Two kinetic phases of Tyro oxidation - the fast phase (msec-sec time range) and the slow phase (tens of seconds time range) were resolved as was previously reported [Vass and Styring (1991) Biochemistry 30, 830]. In the presence of deuterated buffers the kinetics was significantly slower compared to normal buffers. Furthermore, although the kinetics were faster at both high pH and pD values the observed KIE was found to be similar (similar to 2.4) over the whole pL range investigated. We assign the fast and slow oxidation phases to two populations of PSII centers with different water positions, proximal and distal respectively, and discuss possible deprotonation events in the vicinity of Tyro.

    Nyckelord
    Photosystem II, Tyrosine D, Electron transfer, Proton transfer, Deuterium isotope effect
    Nationell ämneskategori
    Biokemi och molekylärbiologi Biofysik
    Identifikatorer
    urn:nbn:se:uu:diva-316938 (URN)10.1016/j.bbabio.2016.11.002 (DOI)000392776400007 ()27823941 (PubMedID)
    Forskningsfinansiär
    Vetenskapsrådet, 621-2013-5937Energimyndigheten, 11674-5Knut och Alice Wallenbergs Stiftelse, KAW 2011.0067
    Tillgänglig från: 2017-03-09 Skapad: 2017-03-09 Senast uppdaterad: 2017-04-30
    2. Tyrosine D oxidation and redox equilibrium in Photosystem II
    Öppna denna publikation i ny flik eller fönster >>Tyrosine D oxidation and redox equilibrium in Photosystem II
    2017 (Engelska)Ingår i: Biochimica et Biophysica Acta - Bioenergetics, ISSN 0005-2728, E-ISSN 1879-2650, Vol. 1858, nr 6, s. 407-417Artikel i tidskrift (Refereegranskat) Published
    Abstract [en]

    Tyrosine ID (Tyr(D)) is an auxiliary redox active tyrosine residue in photosystem II (PSII). The mechanism of Tyr(D) oxidation was investigated by EPR spectroscopy, flash-induced fluorescence decay and thermoluminescence measurements in PSII enriched membranes from spinach. PSII membranes were chemically treated with 3 mM ascorbate and 1 mM diaminodurene and subsequent washing, leading to the complete reduction of Tyr(D). Tyr(D) oxidation kinetics and competing recombination reactions were measured after a single saturating flash in the absence and presence of DCMU (inhibitor of the Q(B)-site) in the pH range of 4.7-8.5. Two kinetic phases of Tyro oxidation were observed by the time resolved EPR spectroscopy the fast phase (msec-sec time range) and the pH dependent slow phase (tens of seconds time range). In the presence of DCMU, Tyr(D) oxidation kinetics was monophasic in the entire pH range, i.e. only the fast kinetics was observed. The results obtained from the fluorescence and thermoluminescence analysis show that when forward electron transport is blocked in the presence of DCMU, the S(2)Q((S) over bar) recombination outcompetes the slow phase of Tyr(D) oxidation by the S-2 state. Modelling of the whole complex of these electron transfer events associated with Tyr(D) oxidation fitted very well with our experimental data. Based on these data, structural information and theoretical considerations we confirm our assignment of the fast and slow oxidation kinetics to two populations of PSII centers with different water positions (proximal and distal) in the Tyr(D) vicinity.

    Nyckelord
    Photosystem II, Electron transfer, Tyrosine D
    Nationell ämneskategori
    Naturvetenskap
    Forskningsämne
    Biokemi
    Identifikatorer
    urn:nbn:se:uu:diva-320913 (URN)10.1016/j.bbabio.2017.02.011 (DOI)000402349000001 ()28235460 (PubMedID)
    Forskningsfinansiär
    Vetenskapsrådet, 621-2013-5937Energimyndigheten, 11674-5Knut och Alice Wallenbergs Stiftelse, 2011.0067
    Tillgänglig från: 2017-04-27 Skapad: 2017-04-27 Senast uppdaterad: 2017-07-06Bibliografiskt granskad
    3. The triplet state of the primary donor, P680, in Photosystem II is not formed by far-red light at 5 K ; Implications for the localization of the primary radical pair.
    Öppna denna publikation i ny flik eller fönster >>The triplet state of the primary donor, P680, in Photosystem II is not formed by far-red light at 5 K ; Implications for the localization of the primary radical pair.
    Visa övriga...
    (Engelska)Manuskript (preprint) (Övrigt vetenskapligt)
    Nyckelord
    Photosystem II, P680, primary charge separation
    Nationell ämneskategori
    Naturvetenskap
    Identifikatorer
    urn:nbn:se:uu:diva-321127 (URN)
    Tillgänglig från: 2017-04-30 Skapad: 2017-04-30 Senast uppdaterad: 2017-05-04
    4. Formation of tyrosine radicals in photosystem II under far-red illumination
    Öppna denna publikation i ny flik eller fönster >>Formation of tyrosine radicals in photosystem II under far-red illumination
    2018 (Engelska)Ingår i: Photosynthesis Research, ISSN 0166-8595, E-ISSN 1573-5079, Vol. 136, nr 1, s. 93-106Artikel i tidskrift (Refereegranskat) Published
    Abstract [en]

    Photosystem II (PS II) contains two redox-active tyrosine residues on the donor side at symmetrical positions to the primary donor, P680. TyrZ, part of the water-oxidizing complex, is a preferential fast electron donor while TyrD is a slow auxiliary donor to P680 +. We used PS II membranes from spinach which were depleted of the water oxidation complex (Mn-depleted PS II) to study electron donation from both tyrosines by time-resolved EPR spectroscopy under visible and far-red continuous light and laser flash illumination. Our results show that under both illumination regimes, oxidation of TyrD occurs via equilibrium with TyrZ at pH 4.7 and 6.3. At pH 8.5 direct TyrD oxidation by P680 + occurs in the majority of the PS II centers. Under continuous far-red light illumination these reactions were less effective but still possible. Different photochemical steps were considered to explain the far-red light-induced electron donation from tyrosines and localization of the primary electron hole (P680 +) on the ChlD1 in Mn-depleted PS II after the far-red light-induced charge separation at room temperature is suggested.

    Nyckelord
    Photosystem II, Tyrosine Z and D, electron transfer
    Nationell ämneskategori
    Biokemi och molekylärbiologi
    Forskningsämne
    Kemi med inriktning mot biofysik
    Identifikatorer
    urn:nbn:se:uu:diva-320914 (URN)10.1007/s11120-017-0442-3 (DOI)000427394300007 ()28924898 (PubMedID)
    Forskningsfinansiär
    Vetenskapsrådet
    Tillgänglig från: 2017-04-27 Skapad: 2017-04-27 Senast uppdaterad: 2018-05-16Bibliografiskt granskad
    5. Role of the PsbTn, a small luminal protein in Photosystem II, in the redox reactions of Tyrosine D
    Öppna denna publikation i ny flik eller fönster >>Role of the PsbTn, a small luminal protein in Photosystem II, in the redox reactions of Tyrosine D
    (Engelska)Manuskript (preprint) (Övrigt vetenskapligt)
    Nyckelord
    Photosystem II, PsbTn, TyrD
    Nationell ämneskategori
    Naturvetenskap
    Identifikatorer
    urn:nbn:se:uu:diva-321125 (URN)
    Tillgänglig från: 2017-04-30 Skapad: 2017-04-30 Senast uppdaterad: 2017-05-04
    6. The Donor-Acceptor side interactions in Photosystem II
    Öppna denna publikation i ny flik eller fönster >>The Donor-Acceptor side interactions in Photosystem II
    (Engelska)Manuskript (preprint) (Övrigt vetenskapligt)
    Nyckelord
    Photosystem II, QA, QB, TyrZ, quinones
    Nationell ämneskategori
    Naturvetenskap
    Forskningsämne
    Biokemi
    Identifikatorer
    urn:nbn:se:uu:diva-321124 (URN)
    Tillgänglig från: 2017-04-30 Skapad: 2017-04-30 Senast uppdaterad: 2017-05-04
  • 19.
    Ahmadova, Nigar
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Molekylär biomimetik.
    Ho, Felix
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Molekylär biomimetik.
    Styring, Stenbjörn
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Molekylär biomimetik.
    Mamedov, Fikret
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Molekylär biomimetik.
    Tyrosine D oxidation and redox equilibrium in Photosystem II2017Ingår i: Biochimica et Biophysica Acta - Bioenergetics, ISSN 0005-2728, E-ISSN 1879-2650, Vol. 1858, nr 6, s. 407-417Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Tyrosine ID (Tyr(D)) is an auxiliary redox active tyrosine residue in photosystem II (PSII). The mechanism of Tyr(D) oxidation was investigated by EPR spectroscopy, flash-induced fluorescence decay and thermoluminescence measurements in PSII enriched membranes from spinach. PSII membranes were chemically treated with 3 mM ascorbate and 1 mM diaminodurene and subsequent washing, leading to the complete reduction of Tyr(D). Tyr(D) oxidation kinetics and competing recombination reactions were measured after a single saturating flash in the absence and presence of DCMU (inhibitor of the Q(B)-site) in the pH range of 4.7-8.5. Two kinetic phases of Tyro oxidation were observed by the time resolved EPR spectroscopy the fast phase (msec-sec time range) and the pH dependent slow phase (tens of seconds time range). In the presence of DCMU, Tyr(D) oxidation kinetics was monophasic in the entire pH range, i.e. only the fast kinetics was observed. The results obtained from the fluorescence and thermoluminescence analysis show that when forward electron transport is blocked in the presence of DCMU, the S(2)Q((S) over bar) recombination outcompetes the slow phase of Tyr(D) oxidation by the S-2 state. Modelling of the whole complex of these electron transfer events associated with Tyr(D) oxidation fitted very well with our experimental data. Based on these data, structural information and theoretical considerations we confirm our assignment of the fast and slow oxidation kinetics to two populations of PSII centers with different water positions (proximal and distal) in the Tyr(D) vicinity.

  • 20.
    Ahmadova, Nigar
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Molekylär biomimetik.
    Mamedov, Fikret
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Molekylär biomimetik.
    Formation of tyrosine radicals in photosystem II under far-red illumination2018Ingår i: Photosynthesis Research, ISSN 0166-8595, E-ISSN 1573-5079, Vol. 136, nr 1, s. 93-106Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Photosystem II (PS II) contains two redox-active tyrosine residues on the donor side at symmetrical positions to the primary donor, P680. TyrZ, part of the water-oxidizing complex, is a preferential fast electron donor while TyrD is a slow auxiliary donor to P680 +. We used PS II membranes from spinach which were depleted of the water oxidation complex (Mn-depleted PS II) to study electron donation from both tyrosines by time-resolved EPR spectroscopy under visible and far-red continuous light and laser flash illumination. Our results show that under both illumination regimes, oxidation of TyrD occurs via equilibrium with TyrZ at pH 4.7 and 6.3. At pH 8.5 direct TyrD oxidation by P680 + occurs in the majority of the PS II centers. Under continuous far-red light illumination these reactions were less effective but still possible. Different photochemical steps were considered to explain the far-red light-induced electron donation from tyrosines and localization of the primary electron hole (P680 +) on the ChlD1 in Mn-depleted PS II after the far-red light-induced charge separation at room temperature is suggested.

  • 21.
    Ahmadova, Nigar
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström.
    Mamedov*, Fikret
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström.
    The Donor-Acceptor side interactions in Photosystem IIManuskript (preprint) (Övrigt vetenskapligt)
  • 22.
    Ahmadova, Nigar
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström.
    Schröder*, Wolfgang P.
    Mamedov, Fikret
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström.
    Role of the PsbTn, a small luminal protein in Photosystem II, in the redox reactions of Tyrosine DManuskript (preprint) (Övrigt vetenskapligt)
  • 23.
    Aitola, Kerttu
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Domanski, Konrad
    Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Lab Photon & Interfaces, CH-1015 Lausanne, Switzerland..
    Correa-Baena, Juan-Pablo
    MIT, 77 Massachusetts Ave, Cambridge, MA 02139 USA..
    Sveinbjörnsson, Kári
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Saliba, Michael
    Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Lab Photon & Interfaces, CH-1015 Lausanne, Switzerland..
    Abate, Antonio
    Univ Fribourg, Adolphe Merkle Inst, CH-1700 Fribourg, Switzerland..
    Graetzel, Michael
    Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Lab Photon & Interfaces, CH-1015 Lausanne, Switzerland..
    Kauppinen, Esko
    Aalto Univ, Dept Appl Phys, POB 15100, Aalto 00076, Finland..
    Johansson, Erik M.J.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Tress, Wolfgang
    Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Lab Photon & Interfaces, CH-1015 Lausanne, Switzerland..
    Hagfeldt, Anders
    Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Lab Photomol Sci, CH-1015 Lausanne, Switzerland..
    Boschloo, Gerrit
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    High Temperature-Stable Perovskite Solar Cell Based on Low-Cost Carbon Nanotube Hole Contact2017Ingår i: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 29, nr 17, artikel-id 1606398Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Mixed ion perovskite solar cells (PSC) are manufactured with a metal-free hole contact based on press-transferred single-walled carbon nanotube (SWCNT) film infiltrated with 2,2,7,-7-tetrakis(N, N-di-p-methoxyphenylamine)-9,90-spirobifluorene (Spiro-OMeTAD). By means of maximum power point tracking, their stabilities are compared with those of standard PSCs employing spin-coated Spiro-OMeTAD and a thermally evaporated Au back contact, under full 1 sun illumination, at 60 degrees C, and in a N-2 atmosphere. During the 140 h experiment, the solar cells with the Au electrode experience a dramatic, irreversible efficiency loss, rendering them effectively nonoperational, whereas the SWCNT-contacted devices show only a small linear efficiency loss with an extrapolated lifetime of 580 h.

  • 24.
    Aitola, Kerttu
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Halme, Janne
    Feldt, Sandra
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Lohse, Peter
    Borghei, Maryam
    Kaskela, Antti
    Nasibulin, Albert G.
    Kauppinen, Esko I.
    Lund, Peter D.
    Boschloo, Gerrit
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Hagfeldt, Anders
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Highly catalytic carbon nanotube counter electrode on plastic for dye solar cells utilizing cobalt-based redox mediator2013Ingår i: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 111, s. 206-209Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    A flexible, slightly transparent and metal-free random network of single-walled carbon nanotubes (SWCNTs) on plain polyethylene terephthalate (PET) plastic substrate outperformed platinum on conductive glass and on plastic as the counter electrode (CE) of a dye solar cell employing a Co(II/III)tris(2,2'-bipyridyl) complex redox mediator in 3-methoxypropionitrile solvent. The CE charge-transfer resistance of the SWCNT film was 0.60 Omega cm(2), 4.0 Omega cm(2) for sputtered platinum on indium tin oxide-PET substrate and 1.7 Omega cm(2) for thermally deposited Pt on fluorine-doped tin oxide glass, respectively. The solar cell efficiencies were in the same range, thus proving that an entirely carbon-based SWCNT film on plastic is as good CE candidate for the Co electrolyte. (C) 2013 Elsevier Ltd. All rights reserved.

  • 25.
    Aitola, Kerttu
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Sveinbjörnsson, Kári
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Correa-Baena, Juan-Pablo
    Ecole Polytech Fed Lausanne, Lab Photomol Sci, EPFL SB ISIC LSPM, CH G1 523,Chemin Alamb,Stn 6, CH-1015 Lausanne, Switzerland..
    Kaskela, Antti
    Aalto Univ, Sch Sci, Dept Appl Phys, POB 15100, FI-00076 Aalto, Finland..
    Abate, Antonio
    Ecole Polytech Fed Lausanne, Lab Photon & Interfaces, Inst Chem Sci & Engn, EPFL SB ISIC LPI, CH G1 526,Stn 6, CH-1015 Lausanne, Switzerland..
    Tian, Ying
    Aalto Univ, Sch Sci, Dept Appl Phys, POB 15100, FI-00076 Aalto, Finland..
    Johansson, Erik M. J.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Graetzel, Michael
    Ecole Polytech Fed Lausanne, Lab Photon & Interfaces, Inst Chem Sci & Engn, EPFL SB ISIC LPI, CH G1 526,Stn 6, CH-1015 Lausanne, Switzerland..
    Kauppinen, Esko I.
    Aalto Univ, Sch Sci, Dept Appl Phys, POB 15100, FI-00076 Aalto, Finland..
    Hagfeldt, Anders
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi. Ecole Polytech Fed Lausanne, Lab Photomol Sci, EPFL SB ISIC LSPM, CH G1 523,Chemin Alamb,Stn 6, CH-1015 Lausanne, Switzerland..
    Boschloo, Gerrit
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Carbon nanotube-based hybrid hole-transporting material and selective contact for high efficiency perovskite solar cells2016Ingår i: Energy & Environmental Science, ISSN 1754-5692, E-ISSN 1754-5706, Vol. 9, nr 2, s. 461-466Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    We demonstrate a high efficiency perovskite solar cell with a hybrid hole-transporting material-counter electrode based on a thin single-walled carbon nanotube (SWCNT) film and a drop-cast 2,2,7,-7-tetrakis(N, N-di-p-methoxyphenylamine)-9,90-spirobifluorene (Spiro-OMeTAD) hole-transporting material (HTM). The average efficiency of the solar cells was 13.6%, with the record cell yielding 15.5% efficiency. The efficiency of the reference solar cells with spin-coated Spiro-OMeTAD hole-transportingmaterials (HTMs) and an evaporated gold counter electrode was 17.7% (record 18.8%), that of the cells with only a SWCNT counter electrode (CE) without additional HTM was 9.1% (record 11%) and that of the cells with gold deposited directly on the perovskite layer was 5% (record 6.3%). Our results show that it is possible to manufacture high efficiency perovskite solar cells with thin film (thickness less than 1 mu m) completely carbon-based HTMCEs using industrially upscalable manufacturing methods, such as press-transferred CEs and drop-cast HTMs.

  • 26.
    Aitola, Kerttu
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Zhang, Jinbao
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Vlachopoulos, Nick
    Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, SB ISIC LSPM, CH-1015 Lausanne, Switzerland..
    Halme, Janne
    Aalto Univ, Sch Sci, Dept Appl Phys, Aalto 00076, Finland..
    Kaskela, Antti
    Aalto Univ, Sch Sci, Dept Appl Phys, Aalto 00076, Finland..
    Nasibulin, Albert G.
    Aalto Univ, Sch Sci, Dept Appl Phys, Aalto 00076, Finland.;Skolkovo Inst Sci & Technol, Skolkovo, Russia..
    Kauppinen, Esko I.
    Aalto Univ, Sch Sci, Dept Appl Phys, Aalto 00076, Finland..
    Boschloo, Gerrit
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Hagfeldt, Anders
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Carbon nanotube film replacing silver in high-efficiency solid-state dye solar cells employing polymer hole conductor2015Ingår i: Journal of Solid State Electrochemistry, ISSN 1432-8488, E-ISSN 1433-0768, Vol. 19, nr 10, s. 3139-3144Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    A semitransparent, flexible single-walled carbon nanotube (SWCNT) film was efficiently used in place of evaporated silver as the counter electrode of a poly(3,4-ethylenedioxythiophene) polymer-based solid-state dye solar cell (SSDSC): the solar-to-electrical energy conversion efficiency of the SWCNT-SSDSC was 4.8 % when it was 5.2 % for the Ag-SSDSC. The efficiency difference stemmed from a 0.1-V difference in the open-circuit voltage, whose reason was speculated to be related to the different recombination processes in the two types of SSDSCs.

  • 27.
    Ajalloueian, F.
    et al.
    Isfahan Univ Technol, Dept Text Engn, Ctr Excellence Appl Nanotechnol, Esfahan, Iran..
    Fransson, M.
    Uppsala universitet, Medicinska och farmaceutiska vetenskapsområdet, Medicinska fakulteten, Institutionen för immunologi, genetik och patologi.
    Tavanai, H.
    Isfahan Univ Technol, Dept Text Engn, Ctr Excellence Appl Nanotechnol, Esfahan, Iran..
    Hilborn, Jöns
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Polymerkemi.
    Magnusson, Peetra
    Uppsala universitet, Medicinska och farmaceutiska vetenskapsområdet, Medicinska fakulteten, Institutionen för immunologi, genetik och patologi, Klinisk immunologi. Uppsala Univ, Dept Immunol Genet & Pathol IGP, Uppsala, Sweden..
    Arpanaei, A.
    Natl Inst Genet Engn & Biotechnol, Dept Ind & Environm Biotechnol, Tehran, Iran..
    Comparing PLGA and PLGA/Chitosan Nanofibers Seeded by Msc: A Cell-scaffold Interaction Study2015Ingår i: Tissue Engineering. Part A, ISSN 1937-3341, E-ISSN 1937-335X, Vol. 21, s. S406-S407Artikel i tidskrift (Övrigt vetenskapligt)
  • 28.
    Ajalloueian, F.
    et al.
    Tech Univ Denmark, Copenhagen, Denmark..
    Hilborn, Jöns
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Polymerkemi.
    Fossum, M.
    Karolinska Inst, Stockholm, Sweden..
    Chronakis, I. S.
    Tech Univ Denmark, Copenhagen, Denmark..
    Integrated Micro/Nanofibrous PLGA-Collagen Scaffold: an Optimized Method for Plastic Compression of Collagen into PLGA Microfibers2015Ingår i: Tissue Engineering. Part A, ISSN 1937-3341, E-ISSN 1937-335X, Vol. 21, s. S347-S347Artikel i tidskrift (Övrigt vetenskapligt)
  • 29.
    Ajalloueian, Fatemeh
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Polymerkemi. Uppsala universitet, Science for Life Laboratory, SciLifeLab.
    Fransson, Moa
    Uppsala universitet, Medicinska och farmaceutiska vetenskapsområdet, Medicinska fakulteten, Institutionen för immunologi, genetik och patologi.
    Tavanai, Hossein
    Massuni, Mohammad
    Hilborn, Jöns
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Polymerkemi. Uppsala universitet, Science for Life Laboratory, SciLifeLab.
    LeBlanc, Katarina
    Arpanaei, Ayyoob
    Magnusson, Peetra
    Uppsala universitet, Medicinska och farmaceutiska vetenskapsområdet, Medicinska fakulteten, Institutionen för immunologi, genetik och patologi, Klinisk immunologi.
    Investigation of Human Mesenchymal Stromal Cells Cultured on PLGA orPLGA/Chitosan Electrospun Nanofibers2015Ingår i: Journal of Bioprocessing & Biotechniques, ISSN 2155-9821, Vol. 5, nr 6, artikel-id 230Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    We compared the viability, proliferation, and differentiation of human Mesenchymal Stromal Cells (MSC)after culture on poly(lactic-co-glycolic acid) (PLGA) and PLGA/chitosan (PLGA/CH) hybrid scaffolds. We appliedconventional and emulsion electrospinning techniques, respectively, for the fabrication of the PLGA and PLGA/CH scaffolds. Electrospinning under optimum conditions resulted in an average fiber diameter of 166 ± 33 nmfor the PLGA/CH and 680 ± 175 nm for the PLGA scaffold. The difference between the tensile strength of thePLGA and PLGA/CH nanofibers was not significant, but PLGA/CH showed a significantly lower tensile modulusand elongation at break. However, it should be noted that the extensibility of the PLGA/CH was higher than thatof the nanofibrous scaffolds of pure chitosan. As expected, a higher degree of hydrophilicity was seen with PLGA/CH, as compared to PLGA alone. The biocompatibility of the PLGA and PLGA/CH scaffolds was compared usingMTS assay as well as analysis by scanning electron microscopy and confocal microscopy. The results showed thatboth scaffold types supported the viability and proliferation of human MSC, with significantly higher rates on PLGA/CH nanofibers. Nonetheless, an analysis of gene expression of MSC grown on either PLGA or PLGA/CH showed asimilar differentiation pattern towards bone, nerve and adipose tissues.

  • 30.
    Ajalloueian, Fatemeh
    et al.
    Tech Univ Denmark, DTU Food, Nanobio Sci Res Grp, Lyngby, Denmark.
    Lemon, Greg
    Karolinska Inst, Dept Clin Sci Intervent & Technol CLINTEC, Stockholm, Sweden.
    Hilborn, Jöns
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Polymerkemi.
    Chronakis, Ioannis S.
    Tech Univ Denmark, DTU Food, Nanobio Sci Res Grp, Lyngby, Denmark.
    Fossum, Magdalena
    Karolinska Inst, Dept Womens & Childrens Hlth, Stockholm, Sweden; Karolinska Inst, Ctr Mol Med, CMM 02, Stockholm, Sweden; Karolinska Univ Hosp, Astrid Lindgren Childrens Hosp, Dept Paediat Surg, Sect Urol, Stockholm, Sweden.
    Bladder biomechanics and the use of scaffolds for regenerative medicine in the urinary bladder2018Ingår i: Nature reviews. Urology, ISSN 1759-4812, E-ISSN 1759-4820, Vol. 15, nr 3, s. 155-174Artikel, forskningsöversikt (Refereegranskat)
    Abstract [en]

    The urinary bladder is a complex organ with the primary functions of storing urine under low and stable pressure and micturition. Many clinical conditions can cause poor bladder compliance, reduced capacity, and incontinence, requiring bladder augmentation or use of regenerative techniques and scaffolds. To replicate an organ that is under frequent mechanical loading and unloading, special attention towards fulfilling its biomechanical requirements is necessary. Several biological and synthetic scaffolds are available, with various characteristics that qualify them for use in bladder regeneration in vitro and in vivo, including in the treatment of clinical conditions. The biomechanical properties of the native bladder can be investigated using a range of mechanical tests for standardized assessments, as well as mathematical and computational bladder biomechanics. Despite a large body of research into tissue engineering of the bladder wall, some features of the native bladder and the scaffolds used to mimic it need further elucidation. Collection of comparable reference data from different animal models would be a helpful tool for researchers and will enable comparison of different scaffolds in order to optimize characteristics before entering preclinical and clinical trials.

  • 31.
    Ajalloueian, Fatemeh
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Polymerkemi.
    Tavanai, Hossein
    Hilborn, Jons
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Polymerkemi.
    Donzel-Gargand, Olivier
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Tekniska sektionen, Institutionen för teknikvetenskaper, Tillämpad materialvetenskap.
    Leifer, Klaus
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Tekniska sektionen, Institutionen för teknikvetenskaper, Tillämpad materialvetenskap.
    Wickham, Abeni
    Arpanaei, Ayyoob
    Emulsion Electrospinning as an Approach to Fabricate PLGA/Chitosan Nanofibers for Biomedical Applications2014Ingår i: BioMed Research International, ISSN 2314-6133, Vol. 2014, s. 475280-Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Novel nanofibers from blends of polylactic-co-glycolic acid (PLGA) and chitosan have been produced through an emulsion electrospinning process. The spinning solution employed polyvinyl alcohol (PVA) as the emulsifier. PVA was extracted from the electrospun nanofibers, resulting in a final scaffold consisting of a blend of PLGA and chitosan. The fraction of chitosan in the final electrospun mat was adjusted from 0 to 33%. Analyses by scanning and transmission electron microscopy show uniform nanofibers with homogenous distribution of PLGA and chitosan in their cross section. Infrared spectroscopy verifies that electrospun mats contain both PLGA and chitosan. Moreover, contact angle measurements show that the electrospun PLGA/chitosanmats are more hydrophilic than electrospun mats of pure PLGA. Tensile strengths of 4.94 MPa and 4.21 MPa for PLGA/chitosan in dry and wet conditions, respectively, illustrate that the polyblend mats of PLGA/chitosan are strong enough for many biomedical applications. Cell culture studies suggest that PLGA/chitosan nanofibers promote fibroblast attachment and proliferation compared to PLGA membranes. It can be assumed that the nanofibrous composite scaffold of PLGA/chitosan could be potentially used for skin tissue reconstruction.

  • 32.
    Ajalloueian, Fatemeh
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Polymerkemi.
    Zeiai, S.
    Fossum, M.
    Hilborn, Jöns
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Polymerkemi.
    A bedside collagen-PLGA nanofibrous construct for autologous transplantation of minced bladder mucosal2012Ingår i: Journal of Tissue Engineering and Regenerative Medicine, ISSN 1932-6254, Vol. 6, nr suppl 1, s. 128-128Artikel i tidskrift (Övrigt vetenskapligt)
    Abstract [en]

    Introduction: Bladder regeneration using minced bladder mucosa is an alternative to costly and time-consuming conventional in vitro culturing of urothelial cells. In this method, the uroepithelium expands in vivo and the patient body appears as an incubator. With our preliminary successes, designing an appropriate scaffold that supports in vivo cell expansion and surgical handling in a clinical setting was our aim. This study, investigates cell expansion in a hybrid construct of collagen/poly (lactic-co-glycolide)(PLGA).

    Materials and methods: An electrospun PLGA mat was placed on a semi-gel collagen inside a mold and covered with a second collagen layer. After gel formation, minced particles of pig bladder mucosa were seeded on the hybrid construct and then processed by plastic compression (PC). The scaffolds were incubated for 2, 4 and 6 weeks in vitro for further studies.

    Results: Tensile tests show an increase in tensile strength of 0.6 ± 0.1 MPa in PC collagen to 3.6 ± 1.1 MPa in hybrid construct. Morphological studies, histological staining and SEM show that the construct has kept its integrity during the time and proliferated urothelial cells have reached confluence after 4 weeks and a multi-layered urothelium after 6 weeks.

    Conclusion: We have designed a mechanically robust scaffold that permits surgical handling and tissue expansion in vivo. The construct is easy-to-use for clinical application in an ordinary surgical operating theater for bladder regeneration.

  • 33.
    Ajalloueian, Fatemeh
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Polymerkemi. Uppsala universitet, Science for Life Laboratory, SciLifeLab.
    Zeiai, Said
    Fossum, Magdalena
    Hilborn, Jöns G.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Polymerkemi. Uppsala universitet, Science for Life Laboratory, SciLifeLab.
    Constructs of electrospun PLGA, compressed collagen and minced urothelium for minimally manipulated autologous bladder tissue expansion2014Ingår i: Biomaterials, ISSN 0142-9612, E-ISSN 1878-5905, Vol. 35, nr 22, s. 5741-5748Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Bladder regeneration based on minced bladder mucosa in vivo expansion is an alternative to in vitro culturing of urothelial cells. Here, we present the design of a hybrid, electrospun poly(lactic-co-glycolide) (PLGA) - plastically compressed (PC) collagen scaffold that could allow in vivo bladder mucosa expansion. Optimisation of electrospinning was performed in order to obtain increased pore sizes and porosity to consolidate the construct and to support neovascularisation and tissue ingrowth. Tensile tests showed an increase in average tensile strength from 0.6 MPa for PC collagen to 3.57 MPa for the hybrid construct. The optimised PLGA support scaffold was placed between two collagen gels, and the minced tissue was distributed either on top or both on top and inside the construct prior to PC; this was then cultured for up to four weeks. Morphology, histology and SEM demonstrated that the construct maintained its integrity throughout cell culture. Cells from minced tissue migrated, expanded and re-organised to a confluent cell layer on the top of the construct after two weeks and formed a multilayered urothelium after four weeks. Cell morphology and phenotype was typical for urothelial mucosa during tissue culture. (C) 2014 Elsevier Ltd. All rights reserved.

  • 34.
    Ajalloueian, Fatemeh
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Polymerkemi.
    Zeiai, Said
    Rojas, Ramiro
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Polymerkemi.
    Fossum, Magdalena
    Hilborn, Jöns
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Polymerkemi.
    One-Stage Tissue Engineering of Bladder Wall Patches for an Easy-To-Use Approach at the Surgical Table2013Ingår i: Tissue Engineering. Part C, Methods, ISSN 1937-3384, E-ISSN 1937-3392, Vol. 19, nr 9, s. 688-696Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    We present a method for producing a cell-scaffold hybrid construct at the bedside. The construct is composed of plastic-compressed collagen together with a poly(e-caprolactone) (PCL)-knitted mesh that yields an integrated, natural-synthetic scaffold. This construct was evaluated by seeding of minced bladder mucosa, followed by proliferation in vitro. High mechanical strength in combination with a biological environment suitable for tissue growth was achieved through the creation of a hybrid construct that showed an increased tensile strength (17.9 +/- 2.6 MPa) when compared to plastic-compressed collagen (0.6 +/- 0.12 MPa). Intimate contact between the collagen and the PCL fabric was required to ensure integrity without delamination of the construct. This contact was achieved by surface alkaline hydrolysis of the PCL, followed by adsorption of poly(vinyl) alcohol. The improvement in hydrophilicity of the PCL-knitted mesh was confirmed through water contact angle measurements, and penetration of the collagen into the mesh was evaluated by scanning electron microscopy (SEM). Particles of minced bladder mucosa tissue were seeded onto this scaffold, and the proliferation was followed for 6 weeks in vitro. Results obtained from phase contrast microscopy, SEM, and histological staining indicated that cells migrated from the minced tissue particles and reorganized on the scaffold. Cells were viable and proliferative, with morphological features characteristic of urothelial cells. Proliferation reached the point at which a multilayer with a resemblance to stratified urothelium was achieved. This successful method could potentially be used for in vivo applications in reconstructive urology as an engineered autologous tissue transplant without the requirement for in vitro culture before transplantation.

  • 35.
    Akkarasamiyo, Sunisa
    et al.
    Stockholm Univ, Dept Organ Chem, S-10691 Stockholm, Sweden..
    Sawadjoon, Supaporn
    Stockholm Univ, Dept Organ Chem, S-10691 Stockholm, Sweden..
    Orthaber, Andreas
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Molekylär biomimetik.
    Samec, Joseph S. M.
    Stockholm Univ, Dept Organ Chem, S-10691 Stockholm, Sweden..
    Tsuji-Trost Reaction of Non-Derivatized Allylic Alcohols2018Ingår i: Chemistry - A European Journal, ISSN 0947-6539, E-ISSN 1521-3765, Vol. 24, nr 14, s. 3488-3498Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Palladium-catalyzed allylic substitution of non-derivatized enantioenriched allylic alcohols with a variety of uncharged N-, S-, C- and O-centered nucleophiles using a bidentate BiPhePhos ligand is described. A remarkable effect of the counter ion (X) of the XPd[kappa(2)-BiPhePhos][kappa(3)-C3H5] was observed. When ClPd[kappa(2)-BiPhePhos][eta(3)-C3H5] (complexI) was used as catalyst, non-reproducible results were obtained. Study of the complex by X-ray crystallography, (PNMR)-P-31 spectroscopy, and ESI-MS showed that a decomposition occurred where one of the phosphite ligands was oxidized to the corresponding phosphate, generating ClPd[kappa(1)-BiPhePhosphite-phosphate][eta(3)-C3H5] species (complexII). When the chloride was exchanged to the weaker coordinating OTf- counter ion the more stable Pd[kappa(2)-BiPhePhos][eta(3)-C3H5](+)+[OTf] (-) (complexIII) was formed. ComplexIII performed better and gave higher enantiospecificities in the substitution reactions. ComplexIII was evaluated in Tsuji-Trost reactions of stereogenic non-derivatized allylic alcohols. The desired products were obtained in good to excellent yields (71-98%) and enantiospecificities (73-99%) for both inter- and intramolecular substitution reactions with only water generated as a by-product. The methodology was applied to key steps in total synthesis of (S)-cuspareine and (+)-lentiginosine. A reaction mechanism involving a palladium hydride as a key intermediate in the activation of the hydroxyl group is proposed in the overall transformation.

  • 36.
    Aktekin, Burak
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    The Electrochemistry of LiNi0.5-xMn1.5+xO4-δ in Li-ion Batteries: Structure, Side-reactions and Cross-talk2019Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
    Abstract [en]

    The use of Li-ion batteries in portable electronic products is today widespread and on-going research is extensively dedicated to improve their performance and energy density for use in electric vehicles. The largest contribution to the overall cell weight comes from the positive electrode material, and improvements regarding this component thereby render a high potential for the development of these types of batteries. A promising candidate is LiNi0.5Mn1.5O4 (LMNO), which offers both high power capability and energy density. However, the instability of conventional electrolytes at the high operating potential (~4.7 V vs. Li+/Li) associated with this electrode material currently prevents its use in commercial applications.

    This thesis work aims to investigate practical approaches which have the potential of overcoming issues related to fast degradation of LNMO-based batteries. This, in turn, necessitates a comprehensive understanding of degradation mechanisms. First, the effect of a well-known electrolyte additive, fluoroethylene carbonate is investigated in LNMO-Li4Ti5O12 (LTO) cells with a focus on the positive electrode. Relatively poor cycling performance is found with 5 wt% additive while 1 wt% additive does not show a significant difference as compared to additive-free electrolytes. Second, a more fundamental study is performed to understand the effect of capacity fading mechanisms contributing to overall cell failure in high-voltage based full-cells. Electrochemical characterization of LNMO-LTO cells in different configurations show how important the electrode interactions (cross-talk) can be for the overall cell behaviour. Unexpectedly fast capacity fading at elevated temperatures is found to originate from a high sensitivity of LTO to cross-talk.

    Third, in situ studies of LNMO are conducted with neutron diffraction and electron microscopy. These show that the oxygen release is not directly related to cation disordering. Moreover, microstructural changes upon heating are observed. These findings suggest new sample preparation strategies, which allow the control of cation disorder without oxygen loss. Following this guidance, ordered and disordered samples with the same oxygen content are prepared. The negative effect of ordering on electrochemical performance is investigated and changes in bulk electronic structure following cycling are found in ordered samples, accompanied by thick surface films on surface and rock-salt phase domains near surface.

    Delarbeten
    1. The Effect of the Fluoroethylene Carbonate Additive in LiNi0.5Mn1.5O4 - Li4Ti5O12 Lithium-Ion Cells
    Öppna denna publikation i ny flik eller fönster >>The Effect of the Fluoroethylene Carbonate Additive in LiNi0.5Mn1.5O4 - Li4Ti5O12 Lithium-Ion Cells
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    2017 (Engelska)Ingår i: Journal of the Electrochemical Society, ISSN 0013-4651, E-ISSN 1945-7111, Vol. 164, nr 4, s. A942-A948Artikel i tidskrift (Refereegranskat) Published
    Abstract [en]

    The effect of the electrolyte additive fluoroethylene carbonate (FEC) for Li-ion batteries has been widely discussed in literature in recent years. Here, the additive is studied for the high-voltage cathode LiNi0.5Mn1.5O4 (LNMO) coupled to Li4Ti5O12 (LTO) to specifically study its effect on the cathode side. Electrochemical performance of full cells prepared by using a standard electrolyte (LP40) with different concentrations of FEC (0, 1 and 5 wt%) were compared and the surface of cycled positive electrodes were analyzed by X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM). The results show that addition of FEC is generally of limited use for this battery system. Addition of 5 wt% FEC results in relatively poor cycling performance, while the cells with 1 wt% FEC showed similar behavior compared to reference cells prepared without FEC. SEM and XPS analysis did not indicate the formation of thick surface layers on the LNMO cathode, however, an increase in layer thickness with increased FEC content in the electrolyte could be observed. XPS analysis on LTO electrodes showed that the electrode interactions between positive and negative electrodes occurred as Mn and Ni were detected on the surface of LTO already after 1 cycle. (C) The Author(s) 2017. Published by ECS. All rights reserved.

    Ort, förlag, år, upplaga, sidor
    ELECTROCHEMICAL SOC INC, 2017
    Nationell ämneskategori
    Kemi
    Identifikatorer
    urn:nbn:se:uu:diva-323509 (URN)10.1149/2.0231706jes (DOI)000400958600056 ()
    Tillgänglig från: 2017-06-14 Skapad: 2017-06-14 Senast uppdaterad: 2019-07-29Bibliografiskt granskad
    2. Understanding the Capacity Loss in LiNi0.5Mn1.5O4-Li4Ti5O12 Lithium-Ion Cells at Ambient and Elevated Temperatures
    Öppna denna publikation i ny flik eller fönster >>Understanding the Capacity Loss in LiNi0.5Mn1.5O4-Li4Ti5O12 Lithium-Ion Cells at Ambient and Elevated Temperatures
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    2018 (Engelska)Ingår i: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 122, nr 21, s. 11234-11248Artikel i tidskrift (Refereegranskat) Published
    Abstract [en]

    The high-voltage spinel LiNi0.5Mn1.5O4, (LNMO) is an attractive positive electrode because of its operating voltage around 4.7 V (vs Li/Li+) and high power capability. However, problems including electrolyte decomposition at high voltage and transition metal dissolution, especially at elevated temperatures, have limited its potential use in practical full cells. In this paper, a fundamental study for LNMO parallel to Li4Ti5O12 (LTO) full cells has been performed to understand the effect of different capacity fading mechanisms contributing to overall cell failure. Electrochemical characterization of cells in different configurations (regular full cells, back-to-back pseudo-full cells, and 3-electrode full cells) combined with an intermittent current interruption technique have been performed. Capacity fade in the full cell configuration was mainly due to progressively limited lithiation of electrodes caused by a more severe degree of parasitic reactions at the LTO electrode, while the contributions from active mass loss from LNMO or increases in internal cell resistance were minor. A comparison of cell formats constructed with and without the possibility of cross-talk indicates that the parasitic reactions on LTO occur because of the transfer of reaction products from the LNMO side. The efficiency of LTO is more sensitive to temperature, causing a dramatic increase in the fading rate at 55 degrees C. These observations show how important the electrode interactions (cross-talk) can be for the overall cell behavior. Additionally, internal resistance measurements showed that the positive electrode was mainly responsible for the increase of resistance over cycling, especially at 55 degrees C. Surface characterization showed that LNMO surface layers were relatively thin when compared with the solid electrolyte interphase (SEI) on LTO. The SEI on LTO does not contribute significantly to overall internal resistance even though these films are relatively thick. X-ray absorption near-edge spectroscopy measurements showed that the Mn and Ni observed on the anode were not in the metallic state; the presence of elemental metals in the SEI is therefore not implicated in the observed fading mechanism through a simple reduction process of migrated metal cations.

    Ort, förlag, år, upplaga, sidor
    American Chemical Society (ACS), 2018
    Nationell ämneskategori
    Materialkemi
    Identifikatorer
    urn:nbn:se:uu:diva-357732 (URN)10.1021/acs.jpcc.8b02204 (DOI)000434236700007 ()
    Forskningsfinansiär
    Energimyndigheten, 42031-1
    Tillgänglig från: 2018-08-31 Skapad: 2018-08-31 Senast uppdaterad: 2019-07-29Bibliografiskt granskad
    3. Cation Ordering and Oxygen Release in LiNi0.5-xMn1.5+xO4-y (LNMO): In Situ Neutron Diffraction and Performance in Li Ion Full Cells
    Öppna denna publikation i ny flik eller fönster >>Cation Ordering and Oxygen Release in LiNi0.5-xMn1.5+xO4-y (LNMO): In Situ Neutron Diffraction and Performance in Li Ion Full Cells
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    2019 (Engelska)Ingår i: ACS APPLIED ENERGY MATERIALS, ISSN 2574-0962, Vol. 2, nr 5, s. 3323-3335Artikel i tidskrift (Refereegranskat) Published
    Abstract [en]

    Lithium ion cells utilizing LiNi0.5Mn1.5O4 (LNMO) as the positive electrode are prone to fast capacity fading, especially when operated in full cells and at elevated temperatures. The crystal structure of LNMO can adopt a P4(3)32 (cation-ordered) or Fd (3) over barm (disordered) arrangement, and the fading rate of cells is usually mitigated when samples possess the latter structure. However, synthesis conditions leading to disordering also lead to oxygen deficiencies and rock-salt impurities and as a result generate Mn3+. In this study, in situ neutron diffraction was performed on disordered and slightly Mn-rich LNMO samples to follow cation ordering-disordering transformations during heating and cooling. The study shows for the first time that there is not a direct connection between oxygen release and cation disordering, as cation disordering is observed to start prior to oxygen release when the samples are heated in a pure oxygen atmosphere. This result demonstrates that it is possible to tune disordering in LNMO without inducing oxygen deficiencies or forming the rock-salt impurity phase. In the second part of the study, electrochemical testing of samples with different degrees of ordering and oxygen content has been performed in LNMO vertical bar vertical bar LTO (Li4Ti5O12) full cells. The disordered sample exhibits better performance, as has been reported in other studies; however, we observe that all cells behave similarly during the initial period of cycling even when discharged at a 10 C rate, while differences arise only after a period of cycling. Additionally, the differences in fading rate were observed to be time-dependent rather than dependent on the number of cycles. This performance degradation is believed to be related to instabilities in LNMO at higher voltages, that is, in its lower lithiation states. Therefore, it is suggested that future studies should target the individual effects of ordering and oxygen content. It is also suggested that more emphasis during electrochemical testing should be placed on the stability of samples in their delithiated state.

    Ort, förlag, år, upplaga, sidor
    AMER CHEMICAL SOC, 2019
    Nyckelord
    high-voltage spinel, neutron diffraction, LNMO, cation ordering, oxygen deficiency
    Nationell ämneskategori
    Materialkemi
    Identifikatorer
    urn:nbn:se:uu:diva-387975 (URN)10.1021/acsaem.8b02217 (DOI)000469885300040 ()
    Forskningsfinansiär
    Energimyndigheten, 42758-1Energimyndigheten, 39043-1StandUp
    Tillgänglig från: 2019-06-27 Skapad: 2019-06-27 Senast uppdaterad: 2019-07-29Bibliografiskt granskad
    4. The role of anionic processes in Li1xNi0.44Mn1.56O4 studied by resonant inelastic X-ray scattering
    Öppna denna publikation i ny flik eller fönster >>The role of anionic processes in Li1xNi0.44Mn1.56O4 studied by resonant inelastic X-ray scattering
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    (Engelska)Manuskript (preprint) (Övrigt vetenskapligt)
    Nationell ämneskategori
    Materialkemi
    Identifikatorer
    urn:nbn:se:uu:diva-389847 (URN)
    Tillgänglig från: 2019-07-29 Skapad: 2019-07-29 Senast uppdaterad: 2019-08-13
    5. How Mn/Ni ordering controls electrochemical performance in high-voltage spinel LiNi0.44Mn1.56O4 (LNMO) with fixed oxygen content
    Öppna denna publikation i ny flik eller fönster >>How Mn/Ni ordering controls electrochemical performance in high-voltage spinel LiNi0.44Mn1.56O4 (LNMO) with fixed oxygen content
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    (Engelska)Manuskript (preprint) (Övrigt vetenskapligt)
    Nyckelord
    High voltage spinel, LNMO, cation ordering, oxygen deficiency, rock-salt, anionic redox activity
    Nationell ämneskategori
    Materialkemi
    Identifikatorer
    urn:nbn:se:uu:diva-389799 (URN)
    Tillgänglig från: 2019-07-28 Skapad: 2019-07-28 Senast uppdaterad: 2019-08-13
  • 37.
    Aktekin, Burak
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Brant, William
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Valvo, Mario
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Marzano, Fernanda
    Scania CV AB.
    Zipprich, Wolfgang
    Volkswagen AG.
    Brandell, Daniel
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Edström, Kristina
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Cation Ordering and Oxygen Release in LiNi0.5-xMn1.5+xO4-y (LNMO)—In Situ Neutron Diffraction and Performance in Li-Ion Full Cells2018Konferensbidrag (Refereegranskat)
    Abstract [en]

    LiNi0.5Mn1.5O4 (LNMO) is a promising spinel-type positive electrode for lithium ion batteries as it operates at high voltage and possesses high power capability. However, rapid performance degradation in full cells, especially at elevated temperatures, is a problem. There has been a considerable interest in its crystal structure as this is known to affect its electrochemical performance. LNMO can adopt a P4332 (cation ordered) or Fd-3m (cation disordered) arrangement depending on the synthesis conditions. Most of the studies in literature agree on better electrochemical performance for disordered LNMO [1], however, a clear understanding of the reason for this behaviour is still lacking. This partly arises from the fact that synthesis conditions leading to disordering also lead to oxygen deficiency, rock-salt impurities and therefore generate some Mn3+ [2]. Most commonly, X-ray diffraction is used to characterize these materials, however, accurate structural analysis is difficult due to the near identical scattering lengths of Mn and Ni. This is not the case for neutron diffraction. In this study, an in-situ neutron diffraction heating-cooling experiment was conducted on slightly Mn-rich LNMO under pure oxygen atmosphere in order to investigate relationship between disordering and oxygen deficiency. The study shows for the first time that there is no direct relationship between oxygen loss and cation disordering, as disordering starts prior to oxygen release. Our findings suggest that it is possible to obtain samples with varying degrees of ordering, yet with the same oxygen content and free from impurities. In the second part of the study, highly ordered, partially ordered and fully disordered samples have been tested in LNMO∥LTO (Li4Ti5O12) full cells at 55 °C. It is shown that differences in their performances arise only after repeated cycling, while all the samples behave similarly at the beginning of the test. The difference is believed to be related to instabilities of LNMO at higher voltages, that is, in its lower lithiation states.

    [1] A. Manthiram, K. Chemelewski, E.-S. Lee, Energy Environ. Sci. 7 (2014) 1339.

    [2] M. Kunduraci, G.G. Amatucci, J. Power Sources. 165 (2007) 359–367.

  • 38.
    Aktekin, Burak
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Lacey, Matthew J.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Nordh, Tim
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Younesi, Reza
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Tengstedt, Carl
    Scania CV AB, SE-15187 Sodertalje, Sweden.
    Zipprich, Wolfgang
    Volkswagen AG, D-38436 Wolfsburg, Germany.
    Brandell, Daniel
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Edström, Kristina
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Understanding the Capacity Loss in LiNi0.5Mn1.5O4-Li4Ti5O12 Lithium-Ion Cells at Ambient and Elevated Temperatures2018Ingår i: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 122, nr 21, s. 11234-11248Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    The high-voltage spinel LiNi0.5Mn1.5O4, (LNMO) is an attractive positive electrode because of its operating voltage around 4.7 V (vs Li/Li+) and high power capability. However, problems including electrolyte decomposition at high voltage and transition metal dissolution, especially at elevated temperatures, have limited its potential use in practical full cells. In this paper, a fundamental study for LNMO parallel to Li4Ti5O12 (LTO) full cells has been performed to understand the effect of different capacity fading mechanisms contributing to overall cell failure. Electrochemical characterization of cells in different configurations (regular full cells, back-to-back pseudo-full cells, and 3-electrode full cells) combined with an intermittent current interruption technique have been performed. Capacity fade in the full cell configuration was mainly due to progressively limited lithiation of electrodes caused by a more severe degree of parasitic reactions at the LTO electrode, while the contributions from active mass loss from LNMO or increases in internal cell resistance were minor. A comparison of cell formats constructed with and without the possibility of cross-talk indicates that the parasitic reactions on LTO occur because of the transfer of reaction products from the LNMO side. The efficiency of LTO is more sensitive to temperature, causing a dramatic increase in the fading rate at 55 degrees C. These observations show how important the electrode interactions (cross-talk) can be for the overall cell behavior. Additionally, internal resistance measurements showed that the positive electrode was mainly responsible for the increase of resistance over cycling, especially at 55 degrees C. Surface characterization showed that LNMO surface layers were relatively thin when compared with the solid electrolyte interphase (SEI) on LTO. The SEI on LTO does not contribute significantly to overall internal resistance even though these films are relatively thick. X-ray absorption near-edge spectroscopy measurements showed that the Mn and Ni observed on the anode were not in the metallic state; the presence of elemental metals in the SEI is therefore not implicated in the observed fading mechanism through a simple reduction process of migrated metal cations.

  • 39.
    Aktekin, Burak
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Lacey, Matthew
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Nordh, Tim
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Tengstedt, Carl
    Scania CV AB.
    Brandell, Daniel
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Edström, Kristina
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Understanding the Rapid Capacity Fading of LNMO-LTO Lithium-ion Cells at Elevated Temperature2017Konferensbidrag (Övrigt vetenskapligt)
    Abstract [en]

    The high voltage spinel LiNi0.5Mn1.5O4 (LNMO) has an average operating potential around 4.7 V vs. Li/Li+ and a gravimetric charge capacity of 146 mAh/g making it a promising high energy density positive electrode for Li-ion batteries. Additionally, the 3-D lithium transport paths available in the spinel structure enables fast diffusion kinetics, making it suitable for power applications [1]. However, the material displays large instability during cycling, especially at elevated temperatures. Therefore, significant research efforts have been undertaken to better understand and improve this electrode material.

    Electrolyte (LiPF6 in organic solvents) oxidation and transition metal dissolution are often considered as the main problems [2] for the systems based on this cathode material. These can cause a variety of problems (in different parts of the cell) eventually increasing internal cell resistance, causing active mass loss and decreasing the amount of cyclable lithium.

    Among these issues, cyclable lithium loss cannot be observed in half cells since lithium metal will provide almost unlimited capacity. Being a promising full cell chemistry for high power applications, there has also been a considerable interest on LNMO full cells with Li4Ti5O12 (LTO) used as the negative electrode. For this chemistry, for an optimized cell, quite stable cycling for >1000 cycles has been reported at room temperature while fast fading is still present at 55 °C [3]. This difference in performance (RT vs. 55 °C) is beyond most expectations and likely does not follow any Arrhenius-type of trend.

    In this study, a comprehensive analysis of LNMO-LTO cells has been performed at different temperatures (RT, 40 °C and 55 °C) to understand the underlying reasons behind stable cycling at room temperature and rapid fading at 55 °C. For this purpose, testing was made on regular cells (Figure 1a), 3-electrode cells (Figure 1b) and back-to-back cells [4] (Figure 1c). Electrode interactions (cross-talk) have been shown to exist in the LTO-LNMO system [5] and back-to-back cells have therefore been used to observe fading under conditions where cross-talk is impossible [4]. Galvanostatic cycling combined with short-duration intermittent current interruptions [6] was performed in order to separately observe changes in internal resistance for LNMO and LTO electrodes in a full cell. Ex-situ characterization of electrodes have also been performed using scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and X-ray absorption near edge spectroscopy (XANES).

    Our findings show how important the electrode interactions can be in full cells, as a decrease in lithium inventory was shown to be the major factor for the observed capacity fading at elevated temperature. In this presentation, the effect of other factors – active mass loss and internal cell resistance – will be discussed together with the consequences of cross-talk.

    References

    [1] A. Kraytsberg et al. Adv. Energy Mater., vol. 2, pp. 922–939,2012.

    [2] J. H. Kim et al., ChemPhysChem, vol. 15, pp. 1940–1954, 2014.

    [3] H. M. Wu et al. J. E. Soc., vol. 156, pp. A1047–A1050, 2009.

    [4] S. R. Li et al., J. E. Soc., vol. 160, no. 9, pp. A1524–A1528, 2013.

    [5] Dedryvère et al. J. Phys. C., vol. 114 (24), pp. 10999–11008, 2010.

    [6] M. J. Lacey, ChemElectroChem, pp. 1–9, 2017.

  • 40.
    Aktekin, Burak
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Lacey, Matthew
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Nordh, Tim
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Younesi, Reza
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Tengstedt, Carl
    Scania CV AB.
    Zipprich, Wolfgang
    Volkswagen AG.
    Brandell, Daniel
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Edström, Kristina
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Understanding the Capacity Loss in LiNi0.5Mn1.5O4 - Li4Ti5O12 Lithium-Ion Cells at Ambient and Elevated Temperatures2017Konferensbidrag (Refereegranskat)
    Abstract [en]

    The high voltage spinel LiNi0.5Mn1.5O(LNMO) is an attractive positive electrode due to its operating voltage around 4.7 V (vs. Li/Li+) arising from the Ni2+/Ni4+ redox couple. In addition to high voltage operation, a second advantage of this material is its capability for fast lithium diffusion kinetics through 3-D transport paths in the spinel structure. However, the electrode material is prone to side reactions with conventional electrolytes, including electrolyte decomposition and transition metal dissolution, especially at elevated temperatures1. It is important to understand how undesired reactions originating from the high voltage spinel affect the aging of different cell components and overall cycle life. Half-cells are usually considered as an ideal cell configuration in order to get information only from the electrode of interest. However, this cell configuration may not be ideal to understand capacity fading for long-term cycling and the assumption of ‘stable’ lithium negative electrode may not be valid, especially at high current rates2. Also, among the variety of capacity fading mechanisms, the loss of “cyclable” lithium from the positive electrode (or gain of lithium from electrolyte into the negative electrode) due to side reactions in a full-cell can cause significant capacity loss. This capacity loss is not observable in a typical half-cell as a result of an excessive reserve of lithium in the negative electrode.

    In a full-cell, it is desired that the negative electrode does not contribute to side reactions in a significant way if the interest is more on the positive side. Among candidates on the negative side, Li4Ti5O12 (LTO) is known for its stability since its voltage plateau (around 1.5 V vs. Li/Li+) is in the electrochemical stability window of standard electrolytes and it shows a very small volume change during lithiation. These characteristics make the LNMO-LTO system attractive for a variety of applications (e.g. electric vehicles) but also make it a good model system for studying aging in high voltage spinel-based full cells.

    In this study, we aim to understand the fundamental mechanisms resulting in capacity fading for LNMO-LTO full cells both at room temperature and elevated temperature (55°C). It is known that electrode interactions occur in this system due to migration of reaction products from LNMO to the LTO side3, 4. For this purpose, three electrode cells have been cycled galvanostatically with short-duration intermittent current interruptionsin order to observe internal resistance for both LNMO and LTO electrodes in a full cell, separately. Change of voltage curves over cycling has also been observed to get an insight into capacity loss. For comparison purposes, back-to-back cells (a combination of LNMO and LTO cells connected electrically by lithium sides) were also tested similarly. Post-cycling of harvested electrodes in half cells was conducted to determine the degree of capacity loss due to charge slippage compared to other aging factors. Surface characterization of LNMO as well as LTO electrodes after cycling at room temperature and elevated temperature has been done via SEM, XPS, HAXPES and XANES.

    References

    1. A. Kraytsberg, Y. Ein-Eli, Adv. Energy Mater., vol. 2, pp. 922–939, 2012.

    2. Aurbach, D., Zinigrad, E., Cohen, Y., & Teller, H. Solid State Ionics, 148(3), 405-416, 2002.

    3. Li et al., Journal of The Electrochemical Society, 160 (9) A1524-A1528, 2013.

    4. Aktekin et al., Journal of The Electrochemical Society 164.4: A942-A948. 2017.

    5. Lacey, M. J., ChemElectroChem. Accepted Author Manuscript. doi:10.1002/celc.201700129, 2017. 

  • 41.
    Aktekin, Burak
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Lacey, Matthew
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Nordh, Tim
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Younesi, Reza
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Tengstedt, Carl
    Scania CV AB.
    Zipprich, Wolfgang
    Volkswagen.
    Brandell, Daniel
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Edström, Kristina
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Understanding the capacity loss in LNMO-LTO lithium-ion cells at ambient and elevated temperaturesManuskript (preprint) (Övrigt vetenskapligt)
    Abstract
  • 42.
    Aktekin, Burak
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Massel, Felix
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Fysiska sektionen, Institutionen för fysik och astronomi, Molekyl- och kondenserade materiens fysik.
    Ahmadi, Majid
    Delft University of Technology, Kavli Institute of Nanoscience, Faculty of Applied Sciences.
    Valvo, Mario
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Hahlin, Maria
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Fysiska sektionen, Institutionen för fysik och astronomi, Molekyl- och kondenserade materiens fysik.
    Zipprich, Wolfgang
    Volkswagen AG.
    Marzano, Fernanda
    Scania CV AB.
    Duda, Laurent
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Fysiska sektionen, Institutionen för fysik och astronomi, Molekyl- och kondenserade materiens fysik.
    Younesi, Reza
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Edström, Kristina
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Brandell, Daniel
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    How Mn/Ni ordering controls electrochemical performance in high-voltage spinel LiNi0.44Mn1.56O4 (LNMO) with fixed oxygen contentManuskript (preprint) (Övrigt vetenskapligt)
  • 43.
    Aktekin, Burak
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Valvo, Mario
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Smith, Ronald I.
    Rutherford Appleton Lab, ISIS Pulsed Neutron & Muon Source, Harwell Campus, Didcot OX11 0QX, Oxon, England.
    Sörby, Magnus H.
    Inst Energy Technol, Dept Neutron Mat Characterizat, POB 40, NO-2027 Kjeller, Norway.
    Marzano, Fernanda Lodi
    Scania CV AB, SE-15187 Sodertalje, Sweden.
    Zipprich, Wolfgang
    Volkswagen AG, D-38436 Wolfsburg, Germany.
    Brandell, Daniel
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Edström, Kristina
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Brant, William
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Cation Ordering and Oxygen Release in LiNi0.5-xMn1.5+xO4-y (LNMO): In Situ Neutron Diffraction and Performance in Li Ion Full Cells2019Ingår i: ACS APPLIED ENERGY MATERIALS, ISSN 2574-0962, Vol. 2, nr 5, s. 3323-3335Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Lithium ion cells utilizing LiNi0.5Mn1.5O4 (LNMO) as the positive electrode are prone to fast capacity fading, especially when operated in full cells and at elevated temperatures. The crystal structure of LNMO can adopt a P4(3)32 (cation-ordered) or Fd (3) over barm (disordered) arrangement, and the fading rate of cells is usually mitigated when samples possess the latter structure. However, synthesis conditions leading to disordering also lead to oxygen deficiencies and rock-salt impurities and as a result generate Mn3+. In this study, in situ neutron diffraction was performed on disordered and slightly Mn-rich LNMO samples to follow cation ordering-disordering transformations during heating and cooling. The study shows for the first time that there is not a direct connection between oxygen release and cation disordering, as cation disordering is observed to start prior to oxygen release when the samples are heated in a pure oxygen atmosphere. This result demonstrates that it is possible to tune disordering in LNMO without inducing oxygen deficiencies or forming the rock-salt impurity phase. In the second part of the study, electrochemical testing of samples with different degrees of ordering and oxygen content has been performed in LNMO vertical bar vertical bar LTO (Li4Ti5O12) full cells. The disordered sample exhibits better performance, as has been reported in other studies; however, we observe that all cells behave similarly during the initial period of cycling even when discharged at a 10 C rate, while differences arise only after a period of cycling. Additionally, the differences in fading rate were observed to be time-dependent rather than dependent on the number of cycles. This performance degradation is believed to be related to instabilities in LNMO at higher voltages, that is, in its lower lithiation states. Therefore, it is suggested that future studies should target the individual effects of ordering and oxygen content. It is also suggested that more emphasis during electrochemical testing should be placed on the stability of samples in their delithiated state.

  • 44.
    Aktekin, Burak
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Younesi, Reza
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Zipprich, Wolfgang
    Volkswagen AG, Wolfsburg, Germany..
    Tengstedt, Carl
    Scania CV AB, Södertalje..
    Brandell, Daniel
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Edström, Kristina
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    The Effect of the Fluoroethylene Carbonate Additive in LiNi0.5Mn1.5O4 - Li4Ti5O12 Lithium-Ion Cells2017Ingår i: Journal of the Electrochemical Society, ISSN 0013-4651, E-ISSN 1945-7111, Vol. 164, nr 4, s. A942-A948Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    The effect of the electrolyte additive fluoroethylene carbonate (FEC) for Li-ion batteries has been widely discussed in literature in recent years. Here, the additive is studied for the high-voltage cathode LiNi0.5Mn1.5O4 (LNMO) coupled to Li4Ti5O12 (LTO) to specifically study its effect on the cathode side. Electrochemical performance of full cells prepared by using a standard electrolyte (LP40) with different concentrations of FEC (0, 1 and 5 wt%) were compared and the surface of cycled positive electrodes were analyzed by X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM). The results show that addition of FEC is generally of limited use for this battery system. Addition of 5 wt% FEC results in relatively poor cycling performance, while the cells with 1 wt% FEC showed similar behavior compared to reference cells prepared without FEC. SEM and XPS analysis did not indicate the formation of thick surface layers on the LNMO cathode, however, an increase in layer thickness with increased FEC content in the electrolyte could be observed. XPS analysis on LTO electrodes showed that the electrode interactions between positive and negative electrodes occurred as Mn and Ni were detected on the surface of LTO already after 1 cycle. (C) The Author(s) 2017. Published by ECS. All rights reserved.

  • 45.
    Aldehani, Mohammed
    et al.
    Univ Lancaster, Dept Engn, Lancaster LA1 4YW, England..
    Alzahrani, Faris
    Univ Lancaster, Dept Engn, Lancaster LA1 4YW, England..
    tSaoir, Meabh Nic An
    Queens Univ Belfast, Sch Chem & Chem Engn, Belfast BT7 1NN, Antrim, North Ireland..
    Fernandes, Daniel Luis Abreu
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Fysikalisk kemi.
    Assabumrungrat, Suttichai
    Chulalongkorn Univ, Fac Engn, Dept Chem Engn, Ctr Excellence Catalysis & Catalyt React Engn, Bangkok, Thailand..
    Aiouache, Farid
    Univ Lancaster, Dept Engn, Lancaster LA1 4YW, England..
    Kinetics and reactive stripping modelling of hydrogen isotopic exchange of deuterated waters2016Ingår i: Chemical Engineering and Processing, ISSN 0255-2701, E-ISSN 1873-3204, Vol. 108, s. 58-73Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    This work presents results of experimental kinetics and modelling of the isotopic exchange between hydrogen and water in a reactive stripping column for water dedeuteriation. The missing physical properties of deuterium and tritium isotopologues in hydrogen gas and water forms were predicted and validated using existing literature data. The kinetic model relevant to a styrene-divinyl-benzene copolymer-supported platinum catalyst was used for modelling, by Aspen plus modular package, impact of design parameters including temperature, total pressure, gas to liquid flowrate ratio, pressure drop and flow mixing, on the separation of deuterium and further the separation of tritium. The modelling by the rate-based non-equilibrium, including design correlations of model of mass and heat transfers, chemical kinetic constants, mass transfer coefficients and overall exchange rate constants, allowed access to separation trends in a good agreement with published data. The synergy between the rates of chemical isotopic exchange and gas/liquid mass transfer, and by inference the performance of reactive stripping, was particularly sensitive to high temperatures, low hydrogen flow rates, pressure drops and internals properties. Extension to tritium confirmed a slightly slower mass transport compared with deuterium leading to potentially under-estimated design features for detritiation processing when deuterium is used instead.

  • 46. Allahverdiyeva, Yagut
    et al.
    Mamedov, Fikret
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström.
    Mäenpää, Pirkko
    Vass, Imre
    Aro, Eva-Mari
    Modulation of photosynthetic electron transport in the absence of terminal electron acceptors: characterization of the rbcL deletion mutant of tobacco2005Ingår i: Biochimica et Biophysica Acta (BBA) - Bioenergetics, ISSN 0005-2728, Vol. 1709, nr 1, s. 69-83Artikel i tidskrift (Refereegranskat)
  • 47.
    Almquist, Martin
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Matematisk-datavetenskapliga sektionen, Institutionen för informationsteknologi, Avdelningen för beräkningsvetenskap. Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Matematisk-datavetenskapliga sektionen, Institutionen för informationsteknologi, Numerisk analys.
    Mattsson, Ken
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Matematisk-datavetenskapliga sektionen, Institutionen för informationsteknologi, Avdelningen för beräkningsvetenskap. Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Matematisk-datavetenskapliga sektionen, Institutionen för informationsteknologi, Numerisk analys.
    Edvinsson, Tomas
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Oorganisk kemi.
    High-fidelity numerical solution of the time-dependent Dirac equation2014Ingår i: Journal of Computational Physics, ISSN 0021-9991, E-ISSN 1090-2716, Vol. 262, s. 86-103Artikel i tidskrift (Refereegranskat)
  • 48.
    Almquist, Martin
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Matematisk-datavetenskapliga sektionen, Institutionen för informationsteknologi, Avdelningen för beräkningsvetenskap. Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Matematisk-datavetenskapliga sektionen, Institutionen för informationsteknologi, Numerisk analys.
    Mattsson, Ken
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Matematisk-datavetenskapliga sektionen, Institutionen för informationsteknologi, Avdelningen för beräkningsvetenskap. Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Matematisk-datavetenskapliga sektionen, Institutionen för informationsteknologi, Numerisk analys.
    Edvinsson, Tomas
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Oorganisk kemi.
    Stable and accurate simulation of phenomena in relativistic quantum mechanics2013Ingår i: Proc. 11th International Conference on Mathematical and Numerical Aspects of Waves, Tunisia: ENIT , 2013, s. 213-214Konferensbidrag (Övrigt vetenskapligt)
  • 49.
    Alvarez Fernandez, Marta
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström.
    Synthesis and Characterization of Iron Complexes, foran Efficient Use in Water Oxidation Catalysis2013Självständigt arbete på grundnivå (kandidatexamen), 10 poäng / 15 hpStudentuppsats (Examensarbete)
  • 50.
    Alvi, Muhammad Rouf
    et al.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Fysikalisk-organisk kemi.
    Jahn, Burkhard O.
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC.
    Tibbelin, Julius
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC.
    Baumgartner, Judith
    Institut für Anorganische Chemie, Technische Universität Graz, Stremayrgasse 9, A-8010 Graz, Austria.
    Gómez, Cesar Pay
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - Ångström, Strukturkemi.
    Ottosson, Henrik
    Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Fysikalisk-organisk kemi.
    Highly Efficient and Convenient Acid Catalyzed Hypersilyl Protection of Alcohols and Thiols by Tris(trimethylsilyl)silyl-N,N-dimethylmethaneamide2012Artikel i tidskrift (Övrigt vetenskapligt)
    Abstract [en]

    Tris(trimethylsilyl)silyl-N,N-dimethylmethaneamide, herein named hypersilylamide, is a convenient and efficient source of the hypersilyl group in the first widely applicable acid catalyzed protocol for silyl group protection of primary, secondary, tertiary alkyl as well as aryl alcohols and thiols in high yields. The sole by-product is N,N-dimethylformamide (DMF) and a range of solvents can be used, including DMF. A high selectivity in the protection of diols can be achieved, also for diols with very small differences in the steric demands at the two hydroxyl groups. Moreover, in the protection of equivalent alcohol and thiol sites the protection of the alcohol is faster, allowing for selective protection in high yields. Quantum chemical calculations at the M062X hybrid meta density functional theory level give insights on the mechanism for the catalytic process. Finally, the hypersilyl group is easily removed from all protected alcohols and thiols examined herein by irradiation at 254 nm.

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