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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 University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, High Energy Physics.
    Bohm, C.
    Bos, F.
    Bose, D.
    Boeser, S.
    Botner, Olga
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, High Energy Physics.
    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 University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, High Energy Physics.
    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 University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, High Energy Physics.
    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 University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, High Energy Physics.
    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 University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, High Energy Physics.
    Strotjohann, N. L.
    Sullivan, G. W.
    Taavola, Henric
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, High Energy Physics.
    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 University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    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 IceCube2015In: European Physical Journal C, ISSN 1434-6044, E-ISSN 1434-6052, Vol. 75, no 3, article id 116Article in journal (Refereed)
    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.

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  • 2.
    Abdelhamid, Hani Nasser
    et al.
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden;Assiut Univ, Dept Chem, Adv Multifunct Mat Lab, Assiut 71515, Egypt.
    El-Zohry, Ahmed M.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Cong, Jiayan
    KTH Royal Inst Technol, Dept Chem, Appl Phys Chem, Tekn Ringen 30, S-10044 Stockholm, Sweden.
    Thersleff, Thomas
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden.
    Karlsson, Martin
    KTH Royal Inst Technol, Dept Chem, Appl Phys Chem, Tekn Ringen 30, S-10044 Stockholm, Sweden.
    Kloo, Lars
    KTH Royal Inst Technol, Dept Chem, Appl Phys Chem, Tekn Ringen 30, S-10044 Stockholm, Sweden.
    Zou, Xiaodong
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden.
    Towards implementing hierarchical porous zeolitic imidazolate frameworks in dye-sensitized solar cells2019In: Royal Society Open Science, E-ISSN 2054-5703, Vol. 6, no 7, article id 190723Article in journal (Refereed)
    Abstract [en]

    A one-pot method for encapsulation of dye, which can be applied for dye-sensitized solar cells (DSSCs), and synthesis of hierarchical porous zeolitic imidazolate frameworks (ZIF-8), is reported. The size of the encapsulated dye tunes the mesoporosity and surface area of ZIF-8. The mesopore size, Langmuir surface area and pore volume are 15 nm, 960-1500 m(2). g(-1) and 0.36-0.61 cm(3). g(-1), respectively. After encapsulation into ZIF-8, the dyes show longer emission lifetimes (greater than 4-8-fold) as compared to the corresponding non-encapsulated dyes, due to suppression of aggregation, and torsional motions.

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  • 3.
    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 University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    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 Molecules2017In: Inorganic Chemistry, ISSN 0020-1669, E-ISSN 1520-510X, Vol. 56, no 15, p. 9139-9146Article in journal (Refereed)
    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).

  • 4.
    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 University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    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 frameworks2019In: Microporous and Mesoporous Materials, ISSN 1387-1811, E-ISSN 1873-3093, Vol. 279, p. 400-406Article in journal (Refereed)
    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.

  • 5.
    Abdellah, Mohamed
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. South Valley Univ, Qena Fac Sci, Dept Chem, Qena 83523, Egypt..
    El-Zohry, Ahmed M.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Antila, Liisa J.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    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 University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Time-Resolved IR Spectroscopy Reveals a. Mechanism with TiO2 as a Reversible Electron Acceptor in a TiO2-Re Catalyst System for CO2 Photoreduction2017In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 139, no 3, p. 1226-1232Article in journal (Refereed)
    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.

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  • 6.
    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 University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    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 dots2017In: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 9, no 34, p. 12503-12508Article in journal (Refereed)
    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.

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  • 7.
    Abdellah, Mohamed
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. 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 University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Competitive Hole Transfer from CdSe Quantum Dots to Thiol Ligands in CdSe-Cobaloxime Sensitized NiO Films Used as Photocathodes for H-2 Evolution2017In: ACS Energy Letters, E-ISSN 2380-8195, Vol. 2, no 11, p. 2576-2580Article in journal (Refereed)
    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.

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  • 8.
    Abdi, Zahra
    et al.
    Inst Adv Studies Basic Sci IASBS, Dept Chem, Zanjan 4513766731, Iran..
    Bagheri, Robabeh
    Soochow Univ, Sch Phys Sci & Technol, Coll Energy, Soochow Inst Energy & Mat Innovat, Suzhou 215006, Peoples R China.;Soochow Univ, Key Lab Adv Carbon Mat & Wearable Energy Technol, Suzhou 215006, Peoples R China..
    Reza Mohammadi, Mohammad
    Univ Sistan & Baluchestan, Dept Phys, Zahedan 9816745845, Iran..
    Song, Zhenlun
    Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Surface Dept, Surface Protect Res Grp, 519 Zhuangshi Rd, Ningbo 315201, Peoples R China..
    Görlin, Mikaela
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Dau, Holger
    Free Univ Berlin, Fachbereich Phys, Arnimallee 14, D-14195 Berlin, Germany..
    Najafpour, Mohammad Mahdi
    Inst Adv Studies Basic Sci IASBS, Dept Chem, Zanjan 4513766731, Iran..
    In Situ Synthesis of Manganese Oxide as an Oxygen-Evolving Catalyst: A New Strategy2021In: Chemistry - A European Journal, ISSN 0947-6539, E-ISSN 1521-3765, Vol. 27, no 4, p. 1330-1336Article in journal (Refereed)
    Abstract [en]

    All studies on oxygen-evolution reaction by Mn oxides in the presence of cerium(IV) ammonium nitrate (CAN) have been so far carried out by synthesizing Mn oxides in the first step. And then, followed by the investigation of the Mn oxides in the presence of oxidants for oxygen-evolution reaction (OER). This paper presents a case study of a new and promising strategy for in situ catalyst synthesis by the adding Mn-II to either CAN or KMnO4/CAN solution, resulting in the formation of Mn-based catalysts for OER. The catalysts were characterized by scanning electron microscopy, energy-dispersive spectroscopy, transmission electron microscopy, X-ray diffraction, Fourier transform infrared spectroscopy, X-ray absorption spectroscopy, and X-ray photoelectron spectroscopy. Both compounds contained nano-sized particles that catalyzed OER in the presence of CAN. The turnover frequencies for both catalysts were 0.02 (mmolO2 /mol(Mn).

  • 9.
    Abdi-Jalebi, Mojtaba
    et al.
    Univ Cambridge, Dept Phys, Cavendish Lab, JJ Thomson Ave, Cambridge, England.
    Pazoki, Meysam
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Philippe, Bertrand
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and Condensed Matter Physics.
    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 University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Lilliu, Samuele
    Univ Sheffield, Dept Phys & Astron, Sheffield, S Yorkshire, England; UAE Ctr Crystallog, Dubai, U Arab Emirates.
    Kullgren, Jolla
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Rensmo, Håkan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and Condensed Matter Physics.
    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 Cations2018In: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 12, no 7, p. 7301-7311Article in journal (Refereed)
    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.

  • 10. Abe, Ryu
    et al.
    Bajada, Mark
    Beller, Matthias
    Bocarsly, Andrew B.
    Butt, Julea N.
    Cassiola, Flavia
    Domcke, Wolfgang
    Durrant, James R.
    Gavrielides, Stelios
    Grätzel, Michael
    Hammarström, Leif
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Hatzell, Marta C.
    König, Burkhard
    Kudo, Akihiko
    Kuehnel, Moritz F.
    Lage, Ava
    Lee, Chong-Yong
    Maneiro, Marcelino
    Minteer, Shelley D.
    Paris, Aubrey R.
    Plumeré, Nicolas
    Reek, Joost N. H.
    Reisner, Erwin
    Roy, Souvik
    Schnedermann, Christoph
    Shankar, Ravi
    Shylin, Sergii I.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Smith, Wilson A.
    Soo, Han Sen
    Wagner, Andreas
    Wielend, Dominik
    Beyond artificial photosynthesis: general discussion2019In: Faraday discussions, ISSN 1359-6640, E-ISSN 1364-5498, Vol. 215, p. 422-438Article in journal (Other (popular science, discussion, etc.))
  • 11.
    Abenayake, Himesha
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Applied Material Science. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.
    Additively Manufactured Rare Earth Free Permanent Magnets2023Independent thesis Advanced level (degree of Master (Two Years)), 20 credits / 30 HE creditsStudent thesis
    Abstract [en]

    It’s well known that MnAl(C) material consists of a metastable phase (τ) with promising ferromagnetic properties, produced either by controlled cooling from the high-temperature hexagonal ε-phase or rapid cooling that freezes the ε-phase followed by low-temperature annealing. Due to the high cooling rates involved, additive manufacturing (AM) especially selective laser melting (SLM), has been identified as a possible method to retain the high-temperature ε-phase, hence containing a potential capacity to produce permanent magnets upon low-temperature annealing. Moreover, the competency of additive manufacturing to address manufacturing design complexity, material scarcity and tailored properties, yields a great opportunity to produce permanent magnets with suitable magnetic properties for complex applications. This work provides a systematic study on three main aspects; development of printing parameters for improved relative density of as-printed MnAl(C) samples; investigation of the influence of scanning strategies on the crystallographic texture of as-printed and annealed samples; investigation of the influence of annealing time and temperature on τ-phase purity and magnetic properties. It was found that laser remelting (multiple laser exposure) combined with specific scanning strategies is a promising path to enhance the relative density of as-printed samples. Some specific scanning strategies were found to be capable of retaining relatively strong crystallographic textured ε-phase in as-printed samples. Following the annealing process for ε→τ transformation, only a partial transformation of crystallographic texture was observed. Characterization of annealed samples through XRD (x-ray diffraction) and phase fractions calculations through Rietveld refinement reveals that relatively short annealing times and low temperatures result in incomplete ε→τ transformation. In addition, longer annealing times and higher temperatures surpass the complete ε→τ transformation and lead to the formation of equilibrium phases subsequently reducing the magnetic performance. Furthermore, the experimental findings demonstrated a pronounced influence of higher carbon content in the powder, resulting in improved magnetic properties.

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    Additively Manufactured Rare Earth Free Permanent Magnets
  • 12. Abi Ghaida, Fatima
    et al.
    Brinkert, Katharina
    Chen, Ping
    DeBeer, Serena
    Hoffman, Brian M.
    Holland, Patrick L.
    Laxmi, Shoba
    MacFarlane, Doug
    Peters, Jonas C.
    Peters, John W.
    Pickett, Christopher J.
    Seefeldt, Lance C.
    Shylin, Sergii I.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Stephens, Ifan E. L.
    Vincent, Kylie A.
    Wang, Qianru
    Westhead, Olivia
    Enzymatic N2 activation: general discussion2023In: Faraday discussions, ISSN 1359-6640, E-ISSN 1364-5498, Vol. 243, p. 287-295Article in journal (Other (popular science, discussion, etc.))
  • 13.
    Ablyasova, Olesya S.
    et al.
    Physikalisches Institut, Albert-Ludwigs-Universität Freiburg, Hermann-Herder-Str. 3, 79104 Freiburg, Germany;Abteilung für Hochempfindliche Röntgenspektroskopie, Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Str. 15, 12489 Berlin, Germany.
    Guo, Meiyuan
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics. SSRL, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States.
    Zamudio-Bayer, Vicente
    Abteilung für Hochempfindliche Röntgenspektroskopie, Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Str. 15, 12489 Berlin, Germany.
    Kubin, Markus
    Abteilung für Hochempfindliche Röntgenspektroskopie, Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Str. 15, 12489 Berlin, Germany.
    Gitzinger, Tim
    Physikalisches Institut, Albert-Ludwigs-Universität Freiburg, Hermann-Herder-Str. 3, 79104 Freiburg, Germany;Abteilung für Hochempfindliche Röntgenspektroskopie, Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Str. 15, 12489 Berlin, Germany.
    da Silva Santos, Mayara
    Physikalisches Institut, Albert-Ludwigs-Universität Freiburg, Hermann-Herder-Str. 3, 79104 Freiburg, Germany;Abteilung für Hochempfindliche Röntgenspektroskopie, Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Str. 15, 12489 Berlin, Germany.
    Flach, Max
    Physikalisches Institut, Albert-Ludwigs-Universität Freiburg, Hermann-Herder-Str. 3, 79104 Freiburg, Germany;Abteilung für Hochempfindliche Röntgenspektroskopie, Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Str. 15, 12489 Berlin, Germany.
    Timm, Martin
    Abteilung für Hochempfindliche Röntgenspektroskopie, Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Str. 15, 12489 Berlin, Germany.
    Lundberg, Marcus
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Lau, J. Tobias
    Physikalisches Institut, Albert-Ludwigs-Universität Freiburg, Hermann-Herder-Str. 3, 79104 Freiburg, Germany;Abteilung für Hochempfindliche Röntgenspektroskopie, Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Str. 15, 12489 Berlin, Germany.
    Hirsch, Konstantin
    Abteilung für Hochempfindliche Röntgenspektroskopie, Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Str. 15, 12489 Berlin, Germany.
    Electronic Structure of the Complete Series of Gas-Phase Manganese Acetylacetonates by X-ray Absorption Spectroscopy2023In: Journal of Physical Chemistry A, ISSN 1089-5639, E-ISSN 1520-5215, Vol. 127, no 34, p. 7121-7131Article in journal (Refereed)
    Abstract [en]

    Metal centers in transition metal–ligand complexes occur in a variety of oxidation states causing their redox activity and therefore making them relevant for applications in physics and chemistry. The electronic state of these complexes can be studied by X-ray absorption spectroscopy, which is, however, due to the complex spectral signature not always straightforward. Here, we study the electronic structure of gas-phase cationic manganese acetylacetonate complexes Mn(acac)1–3+ using X-ray absorption spectroscopy at the metal center and ligand constituents. The spectra are well reproduced by multiconfigurational wave function theory, time-dependent density functional theory as well as parameterized crystal field and charge transfer multiplet simulations. This enables us to get detailed insights into the electronic structure of ground-state Mn(acac)1–3+ and extract empirical parameters such as crystal field strength and exchange coupling from X-ray excitation at both the metal and ligand sites. By comparison to X-ray absorption spectra of neutral, solvated Mn(acac)2,3 complexes, we also show that the effect of coordination on the L3 excitation energy, routinely used to identify oxidation states, can contribute about 40–50% to the observed shift, which for the current study is 1.9 eV per oxidation state.

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  • 14.
    Abrahamsson, Maria
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Becker, Hans-Christian
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Hammarström, Leif
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Microsecond (MLCT)-M-3 excited state lifetimes in bis-tridentate Ru(II)-complexes: significant reductions of non-radiative rate constants2017In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 46, no 39, p. 13314-13321Article in journal (Refereed)
    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.

  • 15.
    Abrashev, Miroslav V.
    et al.
    Univ Sofia St Kliment Ohridski, Fac Phys, Sofia 1164, Bulgaria.
    Chernev, Petko
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics. Free Univ Berlin, Fachbereich Phys, Arnimallee 14, D-14195 Berlin, Germany.
    Kubella, Paul
    Free Univ Berlin, Fachbereich Phys, Arnimallee 14, D-14195 Berlin, Germany.
    Mohammadi, Mohammad Reza
    Free Univ Berlin, Fachbereich Phys, Arnimallee 14, D-14195 Berlin, Germany;Univ Sistan & Baluchestan, Dept Phys, Zahedan 9816745845, Iran.
    Pasquini, Chiara
    Free Univ Berlin, Fachbereich Phys, Arnimallee 14, D-14195 Berlin, Germany.
    Dau, Holger
    Free Univ Berlin, Fachbereich Phys, Arnimallee 14, D-14195 Berlin, Germany.
    Zaharieva, Ivelina
    Free Univ Berlin, Fachbereich Phys, Arnimallee 14, D-14195 Berlin, Germany.
    Origin of the heat-induced improvement of catalytic activity and stability of MnOx electrocatalysts for water oxidation2019In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 7, no 28, p. 17022-17036Article in journal (Refereed)
    Abstract [en]

    Catalysis of the oxygen evolution reaction (OER) by earth-abundant materials in the near-neutral pH regime is of great interest as it is the key reaction for non-fossil fuel production. To address the pertinent stability problems and insufficiently understood structure-activity relations, we investigate the influence of moderate annealing (100-300 degrees C for 20 min) for two types of electrodeposited Mn oxide films with contrasting properties. Upon annealing, the originally inactive and structurally well-ordered Oxide 1 of birnessite type became as OER active as the non-heated Oxide 2, which has a highly disordered atomic structure. Oxide 2 also improved its activity upon heating, but more important is the stability improvement: the operation time increased by about two orders of magnitude (in 0.1 M KPi at pH 7). Aiming at atomistic understanding, electrochemical methods including quantitative analysis of impedance spectra, X-ray spectroscopy (XANES and EXAFS), and adapted optical spectroscopies (infrared, UV-vis and Raman) identified structure-reactivity relations. Oxide structures featuring both di-mu-oxo bridged Mn ions and (close to) linear mono-mu-oxo Mn3+-O-Mn4+ connectivity seem to be a prerequisite for OER activity. The latter motif likely stabilizes Mn3+ ions at higher potentials and promotes electron/hole hopping, a feature related to electrical conductivity and reflected in the strongly accelerated rates of Mn oxidation and O-2 formation. Poor charge mobility, which may result from a low level of Mn3+ ions at high potentials, likely promotes inactivation after prolonged operation. Oxide structures related to the perovskite-like zeta-Mn2O3 were formed after the heating of Oxide 2 and could favour stabilization of Mn ions in oxidation states lower than +4. This rare phase was previously found only at high pressure (20 GPa) and temperature (1200 degrees C) and this is the first report where it was stable under ambient conditions.

  • 16. Achari, Muthuraaman Bhagavathi
    et al.
    Elumalai, Viswanathan
    Vlachopoulos, Nikolaos
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Safdari, Majid
    Gao, Jiajia
    Gardner, James M.
    Kloo, Lars
    A quasi-liquid polymer-based cobalt redox mediator electrolyte for dye-sensitized solar cells2013In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 15, no 40, p. 17419-17425Article in journal (Refereed)
    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.

  • 17. Acker, Pascal
    et al.
    Rzesny, Luisa
    Marchiori, Cleber F. N.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry. Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
    Araujo, Carlos Moyses
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
    Esser, Birgit
    π-Conjugation Enables Ultra-High Rate Capabilities and Cycling Stabilities in Phenothiazine Copolymers as Cathode-Active Battery Materials2019In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 29, no 45, article id 1906436Article in journal (Refereed)
    Abstract [en]

    In recent years, organic battery cathode materials have emerged as an attractive alternative to metal oxide–based cathodes. Organic redox polymers that can be reversibly oxidized are particularly promising. A drawback, however, often is their limited cycling stability and rate performance in a high voltage range of more than 3.4 V versus Li/Li+. Herein, a conjugated copolymer design with phenothiazine as a redox‐active group and a bithiophene co‐monomer is presented, enabling ultra‐high rate capability and cycling stability. After 30 000 cycles at a 100C rate, >97% of the initial capacity is retained. The composite electrodes feature defined discharge potentials at 3.6 V versus Li/Li+ due to the presence of separated phenothiazine redox centers. The semiconducting nature of the polymer allows for fast charge transport in the composite electrode at a high mass loading of 60 wt%. A comparison with three structurally related polymers demonstrates that changing the size, amount, or nature of the side groups leads to a reduced cell performance. This conjugated copolymer design can be used in the development of advanced redox polymers for batteries.

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    fulltext
  • 18.
    Adalsteinsson, Alfred
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Reactions of Li-metal electrodes in contact with electrolytes, characterized by surface analysis techniques2020Independent thesis Advanced level (degree of Master (Two Years)), 20 credits / 30 HE creditsStudent thesis
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    Li_metal_XPS_ALFRED_2020
  • 19.
    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 University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    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 Council2017In: 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, p. 79-92Conference paper (Refereed)
    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.

  • 20. Adamska-Venkatesh, Agnieszka
    et al.
    Mirmohades, Mohammad
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Sommer, Constanze
    Reijerse, Edward
    Lubitz, Wolfgang
    Lomoth, Reiner
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Hammarström, Leif
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Following [FeFe] Hydrogenase Active Site Intermediates by Flash Photolysis/Mid-IR ProbingManuscript (preprint) (Other academic)
  • 21.
    Adolfsson, Karin H. H.
    et al.
    KTH Royal Inst Technol, Dept Fibre & Polymer Technol, S-10044 Stockholm, Sweden..
    Huang, Ping
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Golda-Cepa, Monika
    Jagiellonian Univ, Fac Chem, PL-30387 Krakow, Poland..
    Xu, Huan
    China Univ Min & Technol, Sch Mat Sci & Phys, Xuzhou 221116, Peoples R China..
    Kotarba, Andrzej
    Jagiellonian Univ, Fac Chem, PL-30387 Krakow, Poland..
    Hakkarainen, Minna
    KTH Royal Inst Technol, Dept Fibre & Polymer Technol, S-10044 Stockholm, Sweden..
    Scavenging of DPPH by Persistent Free Radicals in Carbonized Particles2023In: Advanced Sustainable Systems, ISSN 2366-7486, Vol. 7, no 3, article id 2200425Article in journal (Refereed)
    Abstract [en]

    Persistent free radicals (PFR) in carbonized particles may play a role in degradation of environmental compounds. The influence of PFR is evaluated in various carbonized particles on their radical scavenging efficiency upon the common radical indicator 2-2-diphenyl-1-picrylhydrazyl (DPPH). Carbonized particles are derived by hydrothermal carbonization of glucose (C-W) or glucose and urea (NC-W) and ionothermal carbonization of glucose and urea ionic liquid (IL) (NC-IL). The carbonized materials contain OH/COOH, C=C, and C-O functionalities. The addition of urea introduces NH/NH2 functionalities. The content of polar surface groups is lower in IL-processed NC-IL. The scavenging ability, measured as DPPH UV–vis absorption decline, increases with concentration and time for all particles, while the efficiency changes are in the order of C-W > NC-W > NC-IL. Electron paramagnetic resonance analysis reveals similar radical concentration in all carbonized materials studied. The difference in efficiency is, thus, not directly related to the PFR concentration but rather to the type of PFR, surface functionalities and/or scavenging mechanism. According to the g-values, radicals in these particles are carbon-centered. The minor variation in g-values suggests interactions between the radicals and their environmental functional groups. This provides insights into the influence of PFR in carbonized materials on their radical scavenging efficiency.

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  • 22.
    Afewerki, Samson
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Nanotechnology and Functional Materials.
    Wang, Xichi
    Ruiz-Esparza, Guillermo U.
    Tai, Cheuk-Wai
    Kong, Xueying
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Nanotechnology and Functional Materials.
    Zhou, Shengyang
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Nanotechnology and Functional Materials.
    Welch, Ken
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Nanotechnology and Functional Materials.
    Huang, Ping
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Bengtsson, Rhodel
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Applied Mechanics.
    Xu, Chao
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Nanotechnology and Functional Materials.
    Strømme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Nanotechnology and Functional Materials.
    Combined Catalysis for Engineering Bioinspired, Lignin-Based, Long-Lasting, Adhesive, Self-Mending, Antimicrobial Hydrogels2020In: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 14, no 12, p. 17004-17017Article in journal (Refereed)
    Abstract [en]

    The engineering of multifunctional biomaterials using a facile sustainable methodology that follows the principles of green chemistry is still largely unexplored but would be very beneficial to the world. Here, the employment of catalytic reactions in combination with biomass-derived starting materials in the design of biomaterials would promote the development of eco-friendly technologies and sustainable materials. Herein, we disclose the combination of two catalytic cycles (combined catalysis) comprising oxidative decarboxylation and quinone-catechol redox catalysis for engineering lignin-based multifunctional antimicrobial hydrogels. The bioinspired design mimics the catechol chemistry employed by marine mussels in nature. The resultant multifunctional sustainable hydrogels (1) are robust and elastic, (2) have strong antimicrobial activity, (3) are adhesive to skin tissue and various other surfaces, and (4) are able to self-mend. A systematic characterization was carried out to fully elucidate and understand the facile and efficient catalytic strategy and the subsequent multifunctional materials. Electron paramagnetic resonance analysis confirmed the long-lasting quinone-catechol redox environment within the hydrogel system. Initial in vitro biocompatibility studies demonstrated the low toxicity of the hydrogels. This proof-of-concept strategy could be developed into an important technological platform for the eco-friendly, bioinspired design of other multifunctional hydrogels and their use in various biomedical and flexible electronic applications.

  • 23.
    Afroze, Shammya
    et al.
    Univ Brunei Darussalam, Fac Integrated Technol, Jalan Tungku Link, BE-1410 Gadong, Brunei; Chalmers Univ Technol, Dept Chem & Chem Engn, SE-41296 Gothenburg, Sweden..
    Torino, Nico
    Chalmers Univ Technol, Dept Chem & Chem Engn, SE-41296 Gothenburg, Sweden..
    Reza, Md Sumon
    Univ Brunei Darussalam, Fac Integrated Technol, Jalan Tungku Link, BE-1410 Gadong, Brunei..
    Radenahmad, Nikdalila
    Univ Brunei Darussalam, Fac Integrated Technol, Jalan Tungku Link, BE-1410 Gadong, Brunei..
    Cheok, Quentin
    Univ Brunei Darussalam, Fac Integrated Technol, Jalan Tungku Link, BE-1410 Gadong, Brunei..
    Henry, Paul F.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry. Rutherford Appleton Lab, ISIS Pulsed Neutron & Muon Facil, Harwell Campus, Didcot OX11 0QX, Oxon, England..
    Azad, Abul K.
    Univ Brunei Darussalam, Fac Integrated Technol, Jalan Tungku Link, BE-1410 Gadong, Brunei..
    Structure-conductivity relationship of PrBaMnMoO6-δ through in-situ measurements: A neutron diffraction study2021In: Ceramics International, ISSN 0272-8842, E-ISSN 1873-3956, Vol. 47, no 1, p. 541-546Article in journal (Refereed)
    Abstract [en]

    The structural and electrochemical properties of the double perovskite-type oxide, PrBaMnMoO6-δ, was investigated using neutron diffraction with in-situ conductivity measurement under a dry Argon atmosphere from 25 °C to 700 °C. A Rietveld refinement of the neutron diffraction data confirmed monoclinic symmetry in the P21/n space group. Rietveld refinement also confirms the unit cell parameters of a = 5.6567 (1) Å, b = 5.6065 (2) Å, c = 7.9344 (1) Å and β = 84.43° with reliable atomic positions and refinement factors (R-factors). Neutron diffraction data refinement shows two minor phases (< 5%), an orthorhombic AB2O5 type phase of PrMn2O5 in the Pbam (No. 32) space group with unit cell parameters, a = 7.9672 (1) Å, b = 8.9043 (2) Å and c = 5.8540 (1) Å and a scheelite phase of BaMoO4 in the tetragonal I41/a (88) space group with the unit cell parameters, a = b = 5.9522 (1) Å, and c = 12.3211 (2) Å. Morphological images revealed a porous and intertwined microstructure. In-situ conductivity measurement shows that the total conductivity of this material was 130.84 Scm−1 at 700 °C.

  • 24.
    Afroze, Shammya
    et al.
    Univ Brunei Darussalam, Fac Integrated Technol, Jalan Tungku Link, BE-1410 Bandar Seri Begawan, Brunei; Chalmers Univ Technol, Dept Chem & Chem Engn, SE-41296 Gothenburg, Sweden.
    Yilmaz, Duygu
    Chalmers Univ Technol, Dept Chem & Chem Engn, SE-41296 Gothenburg, Sweden.
    Reza, Md Sumon
    Univ Brunei Darussalam, Fac Integrated Technol, Jalan Tungku Link, BE-1410 Bandar Seri Begawan, Brunei.
    Henry, Paul F.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry. Rutherford Appleton Lab, ISIS Pulsed Neutron & Muon Facil, Harwell Campus, Didcot OX11 0QX, Oxon, England.
    Cheok, Quentin
    Univ Brunei Darussalam, Fac Integrated Technol, Jalan Tungku Link, BE-1410 Bandar Seri Begawan, Brunei.
    Zaini, Juliana H.
    Univ Brunei Darussalam, Fac Integrated Technol, Jalan Tungku Link, BE-1410 Bandar Seri Begawan, Brunei.
    Azad, Abul K.
    Univ Brunei Darussalam, Fac Integrated Technol, Jalan Tungku Link, BE-1410 Bandar Seri Begawan, Brunei.
    Issakhov, Alibek
    Al Farabi Kazakh Natl Univ, Dept Math & Comp Modelling, Fac Mech & Math, Alma Ata, Kazakhstan.
    Sadeghzadeh, Milad
    Univ Tehran, Dept Renewable Energy & Environm Engn, Tehran, Iran.
    Investigation of Structural and Thermal Evolution in Novel Layered Perovskite NdSrMn2O5+δ via Neutron Powder Diffraction and Thermogravimetric Analysis2020In: International Journal of Chemical Engineering, ISSN 1687-806X, E-ISSN 1687-8078, Vol. 2020, article id 6642187Article in journal (Refereed)
    Abstract [en]

    Neutron diffraction is one of the best methods for structural analysis of a complex, layered perovskite material with low symmetry by accurately detecting the oxygen positions through octahedral tilting. In this research, the crystal structure of NdSrMn2O5+δ was identified through X-ray diffraction (XRD) and neutron powder diffraction (NPD) at room temperature (RT), which indicated the formation of a layered structure in orthorhombic symmetry in the Pmmm (no. 47) space group. Rietveld refinement of the neutron diffraction data has confirmed the orthorhombic symmetry with unit cell parameters (a = 3.8367 (1) Å, b = 3.8643 (2) Å, and c = 7.7126 (1) Å), atomic positions, and oxygen occupancy. Thermogravimetric analysis revealed the total weight loss of about 0.10% for 20–950°C temperature, which occurred mainly to create oxygen vacancies at high temperatures. Rietveld analyses concurred with the XRD and neutron data allowing correlation of occupancy factors of the oxygen sites.

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  • 25.
    Agarwala, Hemlata
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Synthetic Molecular Chemistry. Tech Univ Munich TUM, Campus Straubing Biotechnol & Sustainabil,Uferstr, D-94315 Straubing, Germany..
    Chen, Xiaoyu
    KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth CBH, Dept Theoret Chem & Biol, S-10691 Stockholm, Sweden..
    Lyonnet, Julien R.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström. Barcelona Inst Sci & Technol, Inst Chem Res Catalonia ICIQ, Tarragona 43007, Spain..
    Johnson, Ben A.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström. Tech Univ Munich TUM, Campus Straubing Biotechnol & Sustainabil,Uferstr, D-94315 Straubing, Germany..
    Ahlquist, Marten
    KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth CBH, Dept Theoret Chem & Biol, S-10691 Stockholm, Sweden..
    Ott, Sascha
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Alternating Metal-Ligand Coordination Improves Electrocatalytic CO2 Reduction by a Mononuclear Ru Catalyst2023In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 62, no 17Article in journal (Refereed)
    Abstract [en]

    Molecular electrocatalysts for CO2-to-CO conversion often operate at large overpotentials, due to the large barrier for C-O bond cleavage. Illustrated with ruthenium polypyridyl catalysts, we herein propose a mechanistic route that involves one metal center that acts as both Lewis base and Lewis acid at different stages of the catalytic cycle, by density functional theory in corroboration with experimental FTIR. The nucleophilic character of the Ru center manifests itself in the initial attack on CO2 to form [Ru-CO2](0), while its electrophilic character allows for the formation of a 5-membered metallacyclic intermediate, [Ru-CO2CO2](0,c), by addition of a second CO2 molecule and intramolecular cyclization. The calculated activation barrier for C-O bond cleavage via the metallacycle is decreased by 34.9 kcal mol(-1) as compared to the non-cyclic adduct in the two electron reduced state of complex 1. Such metallacyclic intermediates in electrocatalytic CO2 reduction offer a new design feature that can be implemented consciously in future catalyst designs.

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  • 26.
    Agervald, Åsa
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Photochemistry and Molecular Science, Microbial Chemistry.
    Camsund, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Stensjö, Karin
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Lindblad, Peter
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    CRISPR in the extended hyp-operon of the cyanobacterium Nostoc sp. strain PCC 7120, characteristics and putative function(s)2012In: International journal of hydrogen energy, ISSN 0360-3199, E-ISSN 1879-3487, Vol. 37, no 10, p. 8828-8833Article in journal (Refereed)
    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.

  • 27.
    Agosta, Lorenzo
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Arismendi-Arrieta, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Dzugutov, Mikhail
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Hermansson, Kersti
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Origin of the Hydrophobic Behaviour of Hydrophilic CeO22023In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 62, no 35, article id e202303910Article in journal (Refereed)
    Abstract [en]

    The nature of the hydrophobicity found in rare-earth oxides is intriguing. The CeO2 (100) surface, despite its strongly hydrophilic nature, exhibits hydrophobic behaviour when immersed in water. In order to understand this puzzling and counter-intuitive effect we performed a detailed analysis of the water structure and dynamics. We report here an ab-initio molecular dynamics simulation (AIMD) study which demonstrates that the first water layer, in immediate contact with the hydroxylated CeO2 surface, is responsible for the effect behaving as a hydrophobic interface with respect to the rest of the liquid water. The hydrophobicity is manifested in several ways: a considerable diffusion enhancement of the confined liquid water as compared with bulk water at the same thermodynamic condition, a weak adhesion energy and few H-bonds above the hydrophobic water layer, which may also sustain a water droplet. These findings introduce a new concept in water/rare-earth oxide interfaces: hydrophobicity mediated by specific water patterns on a hydrophilic surface.

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  • 28.
    Agosta, Lorenzo
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandt, Erik G.
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden..
    Lyubartsev, Alexander
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden..
    Improved Sampling in Ab Initio Free Energy Calculations of Biomolecules at Solid-Liquid Interfaces: Tight-Binding Assessment of Charged Amino Acids on TiO2 Anatase (101)2020In: Computation, E-ISSN 2079-3197, Vol. 8, no 1, article id 12Article in journal (Refereed)
    Abstract [en]

    Atomistic simulations can complement the scarce experimental data on free energies of molecules at bio-inorganic interfaces. In molecular simulations, adsorption free energy landscapes are efficiently explored with advanced sampling methods, but classical dynamics is unable to capture charge transfer and polarization at the solid-liquid interface. Ab initio simulations do not suffer from this flaw, but only at the expense of an overwhelming computational cost. Here, we introduce a protocol for adsorption free energy calculations that improves sampling on the timescales relevant to ab initio simulations. As a case study, we calculate adsorption free energies of the charged amino acids Lysine and Aspartate on the fully hydrated anatase (101) TiO2 surface using tight-binding forces. We find that the first-principle description of the system significantly contributes to the adsorption free energies, which is overlooked by calculations with previous methods.

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  • 29.
    Agosta, Lorenzo
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Dzugutov, Mikhail
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Hermansson, Kersti
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Supercooled liquid-like dynamics in water near a fully hydrated titania surface: Decoupling of rotational and translational diffusion2021In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 154, no 9, article id 094708Article in journal (Refereed)
    Abstract [en]

    We report an ab initio molecular dynamics (MD) simulation investigating the effect of a fully hydrated surface of TiO2 on the water dynamics. It is found that the universal relation between the rotational and translational diffusion characteristics of bulk water is broken in the water layers near the surface with the rotational diffusion demonstrating progressive retardation relative to the translational diffusion when approaching the surface. This kind of rotation-translation decoupling has so far only been observed in the supercooled liquids approaching glass transition, and its observation in water at a normal liquid temperature is of conceptual interest. This finding is also of interest for the application-significant studies of the water interaction with fully hydrated nanoparticles. We note that this is the first observation of rotation-translation decoupling in an ab initio MD simulation of water.

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  • 30.
    Agosta, Lorenzo
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Metere, Alfredo
    Lawrence Livermore Natl Lab, Phys & Life Sci Directorate, Phys Div, Livermore, CA 94550 USA.
    Oleynikov, Peter
    Shanghai Tech Univ, Sch Phys Sci & Technol, Shanghai, Peoples R China.
    Dzugutov, Mikhail
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Self-assembly of a triply periodic continuous mesophase with Fddd symmetry in simple one-component liquids2020In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 152, no 19, article id 191101Article in journal (Refereed)
    Abstract [en]

    Triply periodic continuous morphologies (networks) arising as a result of the microphase separation in block copolymer melts have so far never been observed self-assembled in systems of particles with spherically symmetric interaction. We report a molecular dynamics simulation where two simple one-component liquids form upon cooling an equilibrium network with the Fddd space group symmetry. This complexity reduction in the liquid network formation in terms of the particle geometry and the number of components evidences the generic nature of this class of phase transition, suggesting opportunities for producing these structures in a variety of new systems.

  • 31.
    Aguirre Castillo, José
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.
    Optimisation of the bottom stirring praxis in a LD-LBE converter: Investigations and tests on phosphorous removal, nitrogen as stirring gas, and slopping2015Independent thesis Advanced level (professional degree), 20 credits / 30 HE creditsStudent thesis
    Abstract [en]

    The LD-process, called after the cities Linz and Donawitz, is used to convert pig iron into crude steel by blowing oxygen on top of the pig iron. A LD-LBE converter, Lance Bubbling Equilibrium, also stirs the melt trough a bottom stirring system.

    The bottom stirring in a LD-LBE converter is believed to have a positive effect alone on the phosphorous removal. Previous studies have shown that the temperature and slag composition are the main factors affecting phosphorus removal. Phosphorus binds to the slag easier at low temperature and to slag with certain levels of dissolved calcium (a process additive). Different praxes were tested and a better dephosphorisation was reached. The bottom stirrings effect on the dissolution of calcium additives is a possible explanation to the results and mechanisms presented in this study.

    The study also aimed to investigate the use of nitrogen as stirring gas instead of argon. Nitrogen is removed from the steel during the formation of carbon oxide gases. Nitrogen was used in varying amounts as stirring gas during the first half of the oxygen blow. It proved to be safe to use as long as there was a high content of carbon in the melt. However using nitrogen beyond half of the blow showed to be risky for nitrogen sensible steels; even in small amounts since there is not enough carbon left to degas the steel from nitrogen.

    Slopping happens when formed gas from the LD-process is trapped in the slag. The slag level rises and sometimes it floods the converter resulting in yield losses. The influence of the bottom stirring on slopping was studied, which resulted in the conclusion that slopping cannot be avoided by simply improving the bottom stirring.

    Although some verification studies remains to be done, if the suggestions based on the results of this thesis were employed, savings in the oxygen and stirring gas economies could be made. Not least improvements on the iron yield.

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  • 32.
    Ahlawat, Paramvir
    et al.
    Ecole Polytech Fed Lausanne EPFL, Lab Computat Chem & Biochem, Inst Chem Sci & Engn, CH-1015 Lausanne, Switzerland..
    Hinderhofer, Alexander
    Univ Tubingen, Inst Angew Phys, D-72076 Tubingen, Germany..
    Alharbi, Essa A.
    Ecole Polytech Fed Lausanne, Lab Photon & Interfaces, Inst Chem Sci & Engn, CH-1015 Lausanne, Switzerland..
    Lu, Haizhou
    Ecole Polytech Fed Lausanne, Lab Photon & Interfaces, Inst Chem Sci & Engn, CH-1015 Lausanne, Switzerland.;Ecole Polytech Fed Lausanne, Lab Photomol Sci, Inst Chem Sci Engn, CH-1015 Lausanne, Switzerland..
    Ummadisingu, Amita
    Ecole Polytech Fed Lausanne, Lab Photon & Interfaces, Inst Chem Sci & Engn, CH-1015 Lausanne, Switzerland..
    Niu, Haiyang
    Swiss Fed Inst Technol, Dept Chem & Appl Biosci, CH-8092 Zurich, Switzerland.;Univ Svizzera Italiana, Fac Informat, Ist Sci Computaz, Via G Buffi 13, CH-6900 Lugano, Switzerland..
    Invernizzi, Michele
    Swiss Fed Inst Technol, Dept Chem & Appl Biosci, CH-8092 Zurich, Switzerland.;Univ Svizzera Italiana, Fac Informat, Ist Sci Computaz, Via G Buffi 13, CH-6900 Lugano, Switzerland.;Italian Inst Technol, Via Morego 30, I-16163 Genoa, Italy..
    Zakeeruddin, Shaik Mohammed
    Ecole Polytech Fed Lausanne, Lab Photon & Interfaces, Inst Chem Sci & Engn, CH-1015 Lausanne, Switzerland..
    Dar, M. Ibrahim
    Ecole Polytech Fed Lausanne, Lab Photon & Interfaces, Inst Chem Sci & Engn, CH-1015 Lausanne, Switzerland.;Univ Cambridge, Dept Phys, Cavendish Lab, Cambridge CB3 0HE, England..
    Schreiber, Frank
    Univ Tubingen, Inst Angew Phys, D-72076 Tubingen, Germany..
    Hagfeldt, Anders
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Ecole Polytech Fed Lausanne, Lab Photomol Sci, Inst Chem Sci Engn, CH-1015 Lausanne, Switzerland..
    Graetzel, Michael
    Ecole Polytech Fed Lausanne, Lab Photon & Interfaces, Inst Chem Sci & Engn, CH-1015 Lausanne, Switzerland..
    Rothlisberger, Ursula
    Ecole Polytech Fed Lausanne EPFL, Lab Computat Chem & Biochem, Inst Chem Sci & Engn, CH-1015 Lausanne, Switzerland..
    Parrinello, Michele
    Swiss Fed Inst Technol, Dept Chem & Appl Biosci, CH-8092 Zurich, Switzerland.;Univ Svizzera Italiana, Fac Informat, Ist Sci Computaz, Via G Buffi 13, CH-6900 Lugano, Switzerland.;Italian Inst Technol, Via Morego 30, I-16163 Genoa, Italy..
    A combined molecular dynamics and experimental study of two-step process enabling low-temperature formation of phase-pure alpha-FAPbI32021In: Science Advances, E-ISSN 2375-2548, Vol. 7, no 17, article id eabe3326Article in journal (Refereed)
    Abstract [en]

    It is well established that the lack of understanding the crystallization process in a two-step sequential deposition has a direct impact on efficiency, stability, and reproducibility of perovskite solar cells. Here, we try to understand the solid-solid phase transition occurring during the two-step sequential deposition of methylammonium lead iodide and formamidinium lead iodide. Using metadynamics, x-ray diffraction, and Raman spectroscopy, we reveal the microscopic details of this process. We find that the formation of perovskite proceeds through intermediate structures and report polymorphs found for methylammonium lead iodide and formamidinium lead iodide. From simulations, we discover a possible crystallization pathway for the highly efficient metastable alpha phase of formamidinium lead iodide. Guided by these simulations, we perform experiments that result in the low-temperature crystallization of phase-pure alpha-formamidinium lead iodide.

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  • 33.
    Ahlberg, Patrik
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
    Johansson, Fredrik
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Condensed Matter Physics of Energy Materials.
    Zhang, Zhibin
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
    Jansson, Ulf
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.
    Zhang, Shi-Li
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
    Lindblad, Andreas
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Condensed Matter Physics of Energy Materials.
    Nyberg, Tomas
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
    Defect formation in graphene during low-energy ion bombardment2016In: APL Materials, E-ISSN 2166-532X, Vol. 4, no 4, article id 046104Article in journal (Refereed)
    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.

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  • 34.
    Ahlberg, Patrik
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
    Nyberg, Tomas
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
    Zhang, Shi-Li
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
    Zhang, Zhi-Bin
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
    Jansson, Ulf
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.
    Toward synthesis of oxide films on graphene with sputtering based processes2016In: Journal of Vacuum Science & Technology B, ISSN 1071-1023, E-ISSN 1520-8567, Vol. 34, no 4, article id 040605Article in journal (Refereed)
    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.

  • 35.
    Ahlberg Tidblad, Annika
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström. Volvo Car Corp, SE-40531 Gothenburg, Sweden.
    Edström, Kristina
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Hernández, Guiomar
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    de Meatza, Iratxe
    CIDETEC, Basque Res & Technol Alliance BRTA, P Miramon 196, Donostia San Sebastian 20014, Spain.
    Landa-Medrano, Imanol
    CIDETEC, Basque Res & Technol Alliance BRTA, P Miramon 196, Donostia San Sebastian 20014, Spain.
    Biendicho, Jordi Jacas
    Inst Recerca Energia Catalunya IREC, Barcelona 08930, Spain.
    Trilla, Lluís
    Inst Recerca Energia Catalunya IREC, Barcelona 08930, Spain.
    Buysse, Maarten
    Bax & Co, Barcelona 08013, Spain.
    Ierides, Marcos
    Bax & Co, Barcelona 08013, Spain.
    Perez Horno, Beatriz
    Bax & Co, Barcelona 08013, Spain.
    Kotak, Yash
    TH Ingolstadt, CARISSMA Inst Elect Connected & Secure Mobil C EC, Esplanade 10, D-85049 Ingolstadt, Germany.
    Schweiger, Hans-Georg
    TH Ingolstadt, CARISSMA Inst Elect Connected & Secure Mobil C EC, Esplanade 10, D-85049 Ingolstadt, Germany.
    Koch, Daniel
    TH Ingolstadt, CARISSMA Inst Elect Connected & Secure Mobil C EC, Esplanade 10, D-85049 Ingolstadt, Germany.
    Kotak, Bhavya Satishbhai
    TH Ingolstadt, CARISSMA Inst Elect Connected & Secure Mobil C EC, Esplanade 10, D-85049 Ingolstadt, Germany.
    Future Material Developments for Electric Vehicle Battery Cells Answering Growing Demands from an End-User Perspective2021In: Energies, E-ISSN 1996-1073, Vol. 14, no 14, article id 4223Article, review/survey (Refereed)
    Abstract [en]

    Nowadays, batteries for electric vehicles are expected to have a high energy density, allow fast charging and maintain long cycle life, while providing affordable traction, and complying with stringent safety and environmental standards. Extensive research on novel materials at cell level is hence needed for the continuous improvement of the batteries coupled towards achieving these requirements. This article firstly delves into future developments in electric vehicles from a technology perspective, and the perspective of changing end-user demands. After these end-user needs are defined, their translation into future battery requirements is described. A detailed review of expected material developments follows, to address these dynamic and changing needs. Developments on anodes, cathodes, electrolyte and cell level will be discussed. Finally, a special section will discuss the safety aspects with these increasing end-user demands and how to overcome these issues.

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  • 36.
    Ahlgren, Per
    et al.
    Uppsala University, Disciplinary Domain of Humanities and Social Sciences, Faculty of Social Sciences, Department of Statistics. Uppsala University, University Administration, Planning Division.
    Jeppsson, Tobias
    KTH Biblioteket, KTH Royal Institute of Technology, Stockholm, Sweden.
    Stenberg, Esa
    Uppsala University, University Administration, Faculty Offices.
    Berg, Erik
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Edström, Kristina
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    A bibliometric analysis of battery research with the BATTERY 2030+ roadmap as point of departure2022Report (Other academic)
    Abstract [en]

    In this bibliometric study, we analyze the six battery research subfields identified in the BATTERY 2030+ roadmap: Battery Interface Genome, Materials Acceleration Platform, Recyclability, Smart functionalities: Self-healing, Smart functionalities: Sensing, and Manufacturability. In addition, we analyze the entire research field related to BATTERY 2030+ as a whole, using two operationalizations. We (a) evaluate the European standing in the subfields/the BATTERY 2030+ field in comparison to the rest of the world, and (b) identify strongholds of the subfields/the BATTERY 2030+ field across Europe. For each subfield and the field as a whole, we used seed articles, i.e. articles listed in the BATTERY 2030+ roadmap or cited by such articles, in order to generate additional, similar articles located in an algorithmically obtained classification system. The output of the analysis is publication volumes, field normalized citation impact values with comparisons between country/country aggregates and between organizations, co-publishing networks between countries and organizations, and keyword co-occurrence networks. For the results related to (a), the performance of EU & associated (countries) is similar to China and the aggregate Japan-South Korea-Singapore and well below North America regarding citation impact and with respect to the field as a whole. Exceptions are, however, the subfields Battery Interface Genome and Recyclability. For the results related to (b), there is a large variability in the EU & associated organizations regarding volume in the different subfields. For citation impact, examples of high-performing EU & associated organizations are ETH Zurich and Max Planck Society for the Advancement of Science.

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  • 37.
    Ahlgren, Per
    et al.
    Uppsala University, Disciplinary Domain of Humanities and Social Sciences, Faculty of Social Sciences, Department of Statistics.
    Jeppsson, Tobias
    KTH Royal Inst Technol KTH Lib, KTH Lib, S-10044 Stockholm, Sweden..
    Stenberg, Esa
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Berg, Erik
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Edström, Kristina
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    BATTERY 2030+ and its Research Roadmap: A Bibliometric Analysis2023In: ChemSusChem, ISSN 1864-5631, E-ISSN 1864-564X, Vol. 16, no 21, article id e202300333Article in journal (Refereed)
    Abstract [en]

    In this bibliometric study, we analyze two of the six battery research subfields identified in the BATTERY 2030+ roadmap: Materials Acceleration Platform and Smart functionalities: Sensing. In addition, we analyze the entire research field related to BATTERY 2030+ as a whole. We (a) evaluate the European standing in the two subfields/the BATTERY 2030+ field in comparison to the rest of the world, and (b) identify strongholds of the two subfields/the BATTERY 2030+ field across Europe. For each subfield and the field as a whole, we used seed articles, i. e. articles listed in the BATTERY 2030+ roadmap or cited by such articles, in order to generate additional, similar articles located in an algorithmically obtained classification system. The output of the analysis is publication volumes, field normalized citation impact values with comparisons between country/country aggregates and between organizations, co-publishing networks between countries and organizations, and keyword co-occurrence networks.

    Download full text (pdf)
    fulltext
  • 38.
    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 University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    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 Calculations2017In: Journal of Physical Chemistry A, ISSN 1089-5639, E-ISSN 1520-5215, Vol. 121, no 13, p. 2643-2654Article in journal (Refereed)
    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.

  • 39.
    Ahlstrand, Emma
    et al.
    Linnæus University Centre for Biomaterials Chemistry.
    Spångberg, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Hermansson, Kersti
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Friedman, Ran
    Interaction Energies Between Metal Ions (Zn2+ and Cd2+) and Biologically Relevant Ligands2013In: International Journal of Quantum Chemistry, ISSN 0020-7608, E-ISSN 1097-461X, Vol. 113, no 23, p. 2554-2562Article in journal (Refereed)
    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.

  • 40.
    Ahmadova, Nigar
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Studies of the two redox active tyrosines in Photosystem II2017Doctoral thesis, comprehensive summary (Other academic)
    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.

    List of papers
    1. The protonation state around Tyr(D)/Tyr((D)) over dot in photosystem II is reflected in its biphasic oxidation kinetics
    Open this publication in new window or tab >>The protonation state around Tyr(D)/Tyr((D)) over dot in photosystem II is reflected in its biphasic oxidation kinetics
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    2017 (English)In: Biochimica et Biophysica Acta - Bioenergetics, ISSN 0005-2728, E-ISSN 1879-2650, Vol. 1858, no 2, p. 147-155Article in journal (Refereed) 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.

    Keywords
    Photosystem II, Tyrosine D, Electron transfer, Proton transfer, Deuterium isotope effect
    National Category
    Biochemistry and Molecular Biology Biophysics
    Identifiers
    urn:nbn:se:uu:diva-316938 (URN)10.1016/j.bbabio.2016.11.002 (DOI)000392776400007 ()27823941 (PubMedID)
    Funder
    Swedish Research Council, 621-2013-5937Swedish Energy Agency, 11674-5Knut and Alice Wallenberg Foundation, KAW 2011.0067
    Available from: 2017-03-09 Created: 2017-03-09 Last updated: 2017-04-30
    2. Tyrosine D oxidation and redox equilibrium in Photosystem II
    Open this publication in new window or tab >>Tyrosine D oxidation and redox equilibrium in Photosystem II
    2017 (English)In: Biochimica et Biophysica Acta - Bioenergetics, ISSN 0005-2728, E-ISSN 1879-2650, Vol. 1858, no 6, p. 407-417Article in journal (Refereed) 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.

    Keywords
    Photosystem II, Electron transfer, Tyrosine D
    National Category
    Natural Sciences
    Research subject
    Biochemistry
    Identifiers
    urn:nbn:se:uu:diva-320913 (URN)10.1016/j.bbabio.2017.02.011 (DOI)000402349000001 ()28235460 (PubMedID)
    Funder
    Swedish Research Council, 621-2013-5937Swedish Energy Agency, 11674-5Knut and Alice Wallenberg Foundation, 2011.0067
    Available from: 2017-04-27 Created: 2017-04-27 Last updated: 2017-07-06Bibliographically approved
    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.
    Open this publication in new window or tab >>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.
    Show others...
    (English)Manuscript (preprint) (Other academic)
    Keywords
    Photosystem II, P680, primary charge separation
    National Category
    Natural Sciences
    Identifiers
    urn:nbn:se:uu:diva-321127 (URN)
    Available from: 2017-04-30 Created: 2017-04-30 Last updated: 2017-05-04
    4. Formation of tyrosine radicals in photosystem II under far-red illumination
    Open this publication in new window or tab >>Formation of tyrosine radicals in photosystem II under far-red illumination
    2018 (English)In: Photosynthesis Research, ISSN 0166-8595, E-ISSN 1573-5079, Vol. 136, no 1, p. 93-106Article in journal (Refereed) 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.

    Keywords
    Photosystem II, Tyrosine Z and D, electron transfer
    National Category
    Biochemistry and Molecular Biology
    Research subject
    Chemistry with specialization in Biophysics
    Identifiers
    urn:nbn:se:uu:diva-320914 (URN)10.1007/s11120-017-0442-3 (DOI)000427394300007 ()28924898 (PubMedID)
    Funder
    Swedish Research Council
    Available from: 2017-04-27 Created: 2017-04-27 Last updated: 2018-05-16Bibliographically approved
    5. Role of the PsbTn, a small luminal protein in Photosystem II, in the redox reactions of Tyrosine D
    Open this publication in new window or tab >>Role of the PsbTn, a small luminal protein in Photosystem II, in the redox reactions of Tyrosine D
    (English)Manuscript (preprint) (Other academic)
    Keywords
    Photosystem II, PsbTn, TyrD
    National Category
    Natural Sciences
    Identifiers
    urn:nbn:se:uu:diva-321125 (URN)
    Available from: 2017-04-30 Created: 2017-04-30 Last updated: 2017-05-04
    6. The Donor-Acceptor side interactions in Photosystem II
    Open this publication in new window or tab >>The Donor-Acceptor side interactions in Photosystem II
    (English)Manuscript (preprint) (Other academic)
    Keywords
    Photosystem II, QA, QB, TyrZ, quinones
    National Category
    Natural Sciences
    Research subject
    Biochemistry
    Identifiers
    urn:nbn:se:uu:diva-321124 (URN)
    Available from: 2017-04-30 Created: 2017-04-30 Last updated: 2017-05-04
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  • 41.
    Ahmadova, Nigar
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Ho, Felix
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Styring, Stenbjörn
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Mamedov, Fikret
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Tyrosine D oxidation and redox equilibrium in Photosystem II2017In: Biochimica et Biophysica Acta - Bioenergetics, ISSN 0005-2728, E-ISSN 1879-2650, Vol. 1858, no 6, p. 407-417Article in journal (Refereed)
    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.

  • 42.
    Ahmadova, Nigar
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Mamedov, Fikret
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Formation of tyrosine radicals in photosystem II under far-red illumination2018In: Photosynthesis Research, ISSN 0166-8595, E-ISSN 1573-5079, Vol. 136, no 1, p. 93-106Article in journal (Refereed)
    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.

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  • 43.
    Ahmadova, Nigar
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Mamedov*, Fikret
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    The Donor-Acceptor side interactions in Photosystem IIManuscript (preprint) (Other academic)
  • 44.
    Ahmadova, Nigar
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Schröder*, Wolfgang P.
    Mamedov, Fikret
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Role of the PsbTn, a small luminal protein in Photosystem II, in the redox reactions of Tyrosine DManuscript (preprint) (Other academic)
  • 45.
    Ahmed, Md Estak
    et al.
    Indian Assoc Cultivat Sci, Sch Chem Sci, Kolkata 700032, India..
    Nayek, Abhijit
    Indian Assoc Cultivat Sci, Sch Chem Sci, Kolkata 700032, India..
    Krizan, Alenka
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Coutard, Nathan
    Univ Grenoble Alpes, Lab Chim & Biol Metaux, IRIG, CEA,CNRS, F-38000 Grenoble, France..
    Morozan, Adina
    Univ Grenoble Alpes, Lab Chim & Biol Metaux, IRIG, CEA,CNRS, F-38000 Grenoble, France..
    Dey, Somdatta Ghosh
    Indian Assoc Cultivat Sci, Sch Chem Sci, Kolkata 700032, India..
    Lomoth, Reiner
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Hammarström, Leif
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Artero, Vincent
    Univ Grenoble Alpes, Lab Chim & Biol Metaux, IRIG, CEA,CNRS, F-38000 Grenoble, France..
    Dey, Abhishek
    Indian Assoc Cultivat Sci, Sch Chem Sci, Kolkata 700032, India..
    A Bidirectional Bioinspired [FeFe]-Hydrogenase Model2022In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 144, no 8, p. 3614-3625Article in journal (Refereed)
    Abstract [en]

    With the price-competitiveness of solar and wind power, hydrogen technologies may be game changers for a cleaner, defossilized, and sustainable energy future. H-2 can indeed be produced in electrolyzers from water, stored for long periods, and converted back into power, on demand, in fuel cells. The feasibility of the latter process critically depends on the discovery of cheap and efficient catalysts able to replace platinum group metals at the anode and cathode of fuel cells. Bioinspiration can be key for designing such alternative catalysts. Here we show that a novel class of iron-based catalysts inspired from the active site of [FeFe]-hydrogenase behave as unprecedented bidirectional electrocatalysts for interconverting H-2 and protons efficiently under near-neutral aqueous conditions. Such bioinspired catalysts have been implemented at the anode of a functional membrane-less H-2/O-2 fuel cell device.

  • 46.
    Ahmed, Taha
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Nanostructured ZnO and metal chalcogenide films for solar photocatalysis2023Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    The increasing demand for clean energy and safe water resources has driven the development of efficient and sustainable technologies. Among these technologies, photocatalysis using semiconducting materials has emerged as a promising solution for both solar hydrogen generation and water purification. Low-dimensional ZnO, including nanorods, nanoparticles, and quantum confined particles (so called quantum dots), has demonstrated excellent photocatalytic properties due to their large surface area, high electron mobility, and tunable band gap.

    The work in this thesis aims to investigate the potential of low-dimensional ZnO alone and in combination with CdS and Fe2O3 for solar hydrogen generation and photocatalytic water purification. The thesis includes a comprehensive analysis of the synthesis, characterization, and optimization of low-dimensional ZnO-based photocatalyst systems for solar hydrogen generation and photocatalytic water purification. Additionally, the thesis will evaluate the performance of the ZnO-based photocatalysts under different experimental conditions, either as photoelectrodes or as distributed particle systems for water purification. The work includes detailed size control of ZnO by itself in dimensions below 10 nm using a hydrothermal method, to provide an increased total surface area and introduce quantum confinement effects that increase the band gap to enable degradation of chemical bonds in a model pollutant in a distributed system for water purification. The work also includes a relatively detailed study of the phonon–phonon and electron–phonon coupling as a function of dimension from 10 nm to 150 nm for ZnO using non-resonant and resonant Raman spectroscopy. Ultimately, the thesis aims to provide insight into the potential of low-dimensional ZnO alone and in combination with other inorganic materials for solar hydrogen generation and photocatalytic water purification and pave the way for the development of efficient and sustainable technologies for clean energy and safe water resources.

    List of papers
    1. A facile approach to ZnO/CdS nanoarrays and their photocatalytic and photoelectrochemical properties
    Open this publication in new window or tab >>A facile approach to ZnO/CdS nanoarrays and their photocatalytic and photoelectrochemical properties
    Show others...
    2013 (English)In: Applied Catalysis B: Environmental, ISSN 0926-3373, E-ISSN 1873-3883, Vol. 138, p. 175-183Article in journal (Refereed) Published
    Abstract [en]

    ZnO nanorods were successfully deposited on Transparent Conductive Oxide (TCO) glass by electrochemical deposition, during which initial pulse potential proves important for the fast nucleation and even distribution of ZnO. CdS nanoparticles were coated outside the as-prepared ZnO nanorods by chemical-bath deposition forming ZnO/CdS nanoarrays. The nanoarrays were characterized by X-ray diffraction (XRD), Raman spectroscopy, scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), ultraviolet-visible (UV-vis) spectroscopy, and photoelectrochemistry. The short-circuit current density (J(sc)) of some ZnO/CdS sample showed over 3.3 mA/cm(2) under solar-simulated illumination. The ZnO/CdS nanoarrays showed promising photocatalytic activity with respect to the degradation of Eriochrome Black T (EBT). The relatively high photoelectrochemical properties and photocatalytic performance under visible light irradiation can be ascribed to the enhanced visible light harvest from CdS and charge separation by the coupling of the semiconductors. The combination of electrodeposition and chemical-bath deposition can provide a simple and facile approach to the fabrication of one-dimensional nanocomposites. 

    Keywords
    ZnO, CdS, Nanoarray, Photocatalysis, Photoelectrochemistry
    National Category
    Natural Sciences
    Identifiers
    urn:nbn:se:uu:diva-202887 (URN)10.1016/j.apcatb.2013.02.042 (DOI)000319087900021 ()
    Note

    De två (2) första författarna delar förstaförfattarskapet.

    Available from: 2013-07-01 Created: 2013-07-01 Last updated: 2023-10-30
    2. Preparation and characterisation of ZnO/Fe2O3 core–shell nanorods
    Open this publication in new window or tab >>Preparation and characterisation of ZnO/Fe2O3 core–shell nanorods
    Show others...
    (English)Manuscript (preprint) (Other academic)
    Abstract [en]

    ZnO is a widely used semiconductor photocatalyst. However, the bandgap of ZnO is too large to utilise visible light or solar energy. Therefore, ZnO can couple with a narrow band gap semiconductor that is a visible-light-responsive photocatalyst. ZnO can help with charge seperation through attracting electrons or holes from the other semiconductor. In this work, ZnO nanorods were electrodeposited on FTO glass, and then coated with ultrathin layer of Fe2O3 via ALD.

    SEM, TEM, XPS, Raman and UV-Vis spectroscopies were used to characterise the prepared samples. Raman shows that ALD-coated Fe2O3 is hematite (α-Fe2O3). The prepared ZnO/Fe2O3 shows photocatalytic activity of EBT degradation under visible light illumination. The synthetic strategy can also beextended to prepare other heterostructured photocatalysts.

    National Category
    Inorganic Chemistry
    Identifiers
    urn:nbn:se:uu:diva-515253 (URN)
    Available from: 2023-10-30 Created: 2023-10-30 Last updated: 2023-10-30
    3. Optical Quantum Confinement in Ultrasmall ZnO and the Effect of Size on Their Photocatalytic Activity
    Open this publication in new window or tab >>Optical Quantum Confinement in Ultrasmall ZnO and the Effect of Size on Their Photocatalytic Activity
    2020 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 124, no 11, p. 6395-6404Article in journal (Refereed) Published
    Abstract [en]

    Zinc oxide is a well-known metal oxide semiconductor with a wide direct band gap that offers a promising alternative to titanium oxide in photocatalytic applications. ZnO is studied here as quantum dots (QDs) in colloidal suspensions, where ultrasmall nanoparticles of ZnO show optical quantum confinement with a band gap opening for particles below 9 nm in diameter from the shift of the band edge energies. The optical properties of growing ZnO QDs are determined with Tauc analysis, and a system of QDs for the treatment and degradation of distributed threats is analyzed using an organic probe molecule, methylene blue, whose UV/vis spectrum is analyzed in some detail. The effect of optical properties of the QDs and the kinetics of dye degradation are quantified for low-dimensional ZnO materials in the range of 3-8 nm and show a substantial increase in photocatalytic activity compared to larger ZnO particles. This is attributed to a combined effect from the increased surface area as well as a quantum confinement effect that goes beyond the increased surface area. The results show a significantly higher photocatalytic activity for the QDs between 3 and 6 nm with a complete decolorization of the organic probe molecule, while QDs from 6 nm and upward in diameter show signs of competing reduction reactions. Our study shows that ultrasmall ZnO particles have a reactivity beyond that which is expected because of their increased surface area and also demonstrates size-dependent reaction pathways, which introduces the possibility for size-selective catalysis.

    Place, publisher, year, edition, pages
    AMER CHEMICAL SOC, 2020
    National Category
    Physical Chemistry Theoretical Chemistry
    Identifiers
    urn:nbn:se:uu:diva-410900 (URN)10.1021/acs.jpcc.9b11229 (DOI)000526396000057 ()
    Funder
    Swedish Research Council Formas, 2016-00908
    Available from: 2020-05-25 Created: 2020-05-25 Last updated: 2023-10-30Bibliographically approved
    4. Phonon–phonon and electron–phonon coupling in nano-dimensional ZnO
    Open this publication in new window or tab >>Phonon–phonon and electron–phonon coupling in nano-dimensional ZnO
    Show others...
    (English)Manuscript (preprint) (Other academic)
    Abstract [en]

    Thermal losses through vibrational coupling are critical bottlenecks limiting several materials classes from reaching their full potential. Altering the phonon–phonon and electron–phonon coupling by controlled suppression of vibrational degrees of freedom through low-dimensionality are promising but still largely unexplored approaches. Here we report a detailed study of the first- and second-order Raman processes as a function of size for low-dimensional ZnO. Wurtzite ZnO nanoparticles were synthesised into 3D frameworks of ZnO crystallites, with tailored crystallite diameters from 10 nm to 150 nm and characterised by electron microscopy, X-ray diffraction and non-resonant and resonant Raman spectroscopy.

    We present a short derivation of how resonance Raman and the relation between the longitudinal optical (LO) phonons can be utilised to quantify the electron–phonon coupling, its merits, and limitations. Theoretical Raman response using density functional theory is corroborating the experimental data in assigning first- and second-order Raman modes. The Lyddane-Sachs-Teller equation was applied to the measured LO–TO split and revealed no change in the ratio between the static and high-frequency dielectric constant with changing ZnO dimension from 10 nm to 150 nm. The second-order Raman revealed a phonon–phonon coupling that generally increased with particle size and markedly so for differential modes. Resonance Raman showed the fundamental LO mode and the 2nd, 3rd, and 4th overtones. The intensity relation between the fundamental LO mode and its overtones enabled the extraction of the change in electron–phonon coupling via the Huang-Rhys parameter as a function of particle size, which showed an increase with particle size.

    National Category
    Physical Chemistry
    Identifiers
    urn:nbn:se:uu:diva-515256 (URN)
    Available from: 2023-10-30 Created: 2023-10-30 Last updated: 2023-10-30
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  • 47.
    Ahmed, Taha
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Edvinsson, Tomas
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Solid State Physics.
    Optical Quantum Confinement in Ultrasmall ZnO and the Effect of Size on Their Photocatalytic Activity2020In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 124, no 11, p. 6395-6404Article in journal (Refereed)
    Abstract [en]

    Zinc oxide is a well-known metal oxide semiconductor with a wide direct band gap that offers a promising alternative to titanium oxide in photocatalytic applications. ZnO is studied here as quantum dots (QDs) in colloidal suspensions, where ultrasmall nanoparticles of ZnO show optical quantum confinement with a band gap opening for particles below 9 nm in diameter from the shift of the band edge energies. The optical properties of growing ZnO QDs are determined with Tauc analysis, and a system of QDs for the treatment and degradation of distributed threats is analyzed using an organic probe molecule, methylene blue, whose UV/vis spectrum is analyzed in some detail. The effect of optical properties of the QDs and the kinetics of dye degradation are quantified for low-dimensional ZnO materials in the range of 3-8 nm and show a substantial increase in photocatalytic activity compared to larger ZnO particles. This is attributed to a combined effect from the increased surface area as well as a quantum confinement effect that goes beyond the increased surface area. The results show a significantly higher photocatalytic activity for the QDs between 3 and 6 nm with a complete decolorization of the organic probe molecule, while QDs from 6 nm and upward in diameter show signs of competing reduction reactions. Our study shows that ultrasmall ZnO particles have a reactivity beyond that which is expected because of their increased surface area and also demonstrates size-dependent reaction pathways, which introduces the possibility for size-selective catalysis.

  • 48.
    Ahmed, Taha
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Fondell, Mattis
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Donzel-Gargand, Olivier
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Solar Cell Technology.
    Boman, Mats
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.
    Zhu, Jiefang
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Preparation and characterisation of ZnO/Fe2O3 core–shell nanorodsManuscript (preprint) (Other academic)
    Abstract [en]

    ZnO is a widely used semiconductor photocatalyst. However, the bandgap of ZnO is too large to utilise visible light or solar energy. Therefore, ZnO can couple with a narrow band gap semiconductor that is a visible-light-responsive photocatalyst. ZnO can help with charge seperation through attracting electrons or holes from the other semiconductor. In this work, ZnO nanorods were electrodeposited on FTO glass, and then coated with ultrathin layer of Fe2O3 via ALD.

    SEM, TEM, XPS, Raman and UV-Vis spectroscopies were used to characterise the prepared samples. Raman shows that ALD-coated Fe2O3 is hematite (α-Fe2O3). The prepared ZnO/Fe2O3 shows photocatalytic activity of EBT degradation under visible light illumination. The synthetic strategy can also beextended to prepare other heterostructured photocatalysts.

  • 49.
    Ahmed, Taha
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Thyr, Jakob
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Solid State Physics.
    Naim Katea, Sarmad
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.
    Westin, Gunnar
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.
    Edvinsson, Tomas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry. Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Solid State Physics. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Phonon–phonon and electron–phonon coupling in nano-dimensional ZnOManuscript (preprint) (Other academic)
    Abstract [en]

    Thermal losses through vibrational coupling are critical bottlenecks limiting several materials classes from reaching their full potential. Altering the phonon–phonon and electron–phonon coupling by controlled suppression of vibrational degrees of freedom through low-dimensionality are promising but still largely unexplored approaches. Here we report a detailed study of the first- and second-order Raman processes as a function of size for low-dimensional ZnO. Wurtzite ZnO nanoparticles were synthesised into 3D frameworks of ZnO crystallites, with tailored crystallite diameters from 10 nm to 150 nm and characterised by electron microscopy, X-ray diffraction and non-resonant and resonant Raman spectroscopy.

    We present a short derivation of how resonance Raman and the relation between the longitudinal optical (LO) phonons can be utilised to quantify the electron–phonon coupling, its merits, and limitations. Theoretical Raman response using density functional theory is corroborating the experimental data in assigning first- and second-order Raman modes. The Lyddane-Sachs-Teller equation was applied to the measured LO–TO split and revealed no change in the ratio between the static and high-frequency dielectric constant with changing ZnO dimension from 10 nm to 150 nm. The second-order Raman revealed a phonon–phonon coupling that generally increased with particle size and markedly so for differential modes. Resonance Raman showed the fundamental LO mode and the 2nd, 3rd, and 4th overtones. The intensity relation between the fundamental LO mode and its overtones enabled the extraction of the change in electron–phonon coupling via the Huang-Rhys parameter as a function of particle size, which showed an increase with particle size.

  • 50. Aitchison, Catherine M.
    et al.
    Andrei, Virgil
    Antón-García, Daniel
    Apfel, Ulf-Peter
    Badiani, Vivek
    Beller, Matthias
    Bocarsly, Andrew B.
    Bonnet, Sylvestre
    Brueggeller, Peter
    Caputo, Christine A.
    Cassiola, Flavia
    Clausing, Simon T.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Synthetic Molecular Chemistry.
    Cooper, Andrew I.
    Creissen, Charles E.
    de la Peña O’Shea, Víctor A.
    Domcke, Wolfgang
    Durrant, James R.
    Grätzel, Michael
    Hammarström, Leif
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Hankin, Anna
    Hatzell, Marta C.
    Karadas, Ferdi
    König, Burkhard
    Kuehnel, Moritz F.
    Lamaison, Sarah
    Lin, Chia-Yu
    Maneiro, Marcelino
    Minteer, Shelley D.
    R. Paris, Aubrey
    Pastor, Ernest
    Pornrungroj, Chanon
    Reek, Joost N. H.
    Reisner, Erwin
    Roy, Souvik
    Sahm, Constantin
    Shankar, Ravi
    Shaw, Wendy J.
    Shylin, Sergii I.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Smith, Wilson A.
    Sokol, Katarzyna
    Soo, Han Sen
    Sprick, Reiner Sebastian
    Viertl, Wolfgang
    Vogel, Anastasia
    Wagner, Andreas
    Wakerley, David
    Wang, Qian
    Wielend, Dominik
    Zwijnenburg, Martijn A.
    Synthetic approaches to artificial photosynthesis: general discussion2019In: Faraday discussions, ISSN 1359-6640, E-ISSN 1364-5498, Vol. 215, p. 242-281Article in journal (Other academic)
1234567 1 - 50 of 4512
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