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  • 51.
    Pullen, Sonja
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics. TU Dortmund Univ, Fac Chem & Chem Biol, Otto Hahn Str 6, D-44227 Dortmund, Germany.
    Maji, Somnath
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics. Indian Inst Technol Hyderabad, Dept Chem, Sangareddy 502285, Telangana, India.
    Stein, Matthias
    Max Planck Inst Dynam Complex Tech Syst, Sandtorstr 2, D-39106 Magdeburg, Germany.
    Ott, Sascha
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Restricted rotation of an Fe(CO)(2)(PL3)-subunit in [FeFe]-hydrogenase active site mimics by intramolecular ligation2019In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 48, no 18, p. 5933-5939Article in journal (Refereed)
    Abstract [en]

    A new series of homodinuclear iron complexes as models of the [FeFe]-hydrogenase active site was prepared and characterized. The complexes of the general formula [Fe-2(mcbdt)(CO)(5)PPh2R] (mcbdt = benzene-1,2-dithiol-3-carboxylic acid) feature covalent tethers that link the mcbdt ligand with the phosphine ligands which are terminally coordinated to one of the Fe centres. The synthetic feasability of the concept is demonstrated with the preparation of three novel complexes. A detailed theoretical investigation showes that by introducing a rigid covalent link between the phosphine and the bridging dithiolate ligands, the rotation of the Fe(CO)(2)P unit is hindered and higher rotation barriers were calculated compared to non-linked reference complexes. The concept of restricting Fe(L)(3) rotation is an approach to kinetically stabilize terminal hydrides which are reactive intermediates in catalytic proton reduction cycles of the enzymes.

  • 52.
    Safdari, Rasoul
    et al.
    IASBS, Dept Chem, Zanjan 4513766731, Iran.
    Mohammadi, Mohammad Reza
    Free Univ Berlin, Fachbereich Phys, Arnimallee 14, D-14195 Berlin, Germany;Univ Sistan & Baluchestan, Dept Phys, Zahedan 9816745845, Iran.
    Holynska, Malgorzata
    Philipps Univ Marburg, Fachbereich Chem, Hans Meerwein Str, D-35032 Marburg, Germany;Philipps Univ Marburg, WZMW, Hans Meerwein Str, D-35032 Marburg, Germany.
    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.
    Dau, Holger
    Free Univ Berlin, Fachbereich Phys, Arnimallee 14, D-14195 Berlin, Germany.
    Najafpour, Mohammad Mahdi
    IASBS, Dept Chem, Zanjan 4513766731, Iran;IASBS, Ctr Climate Change & Global Warming, Zanjan 4513766731, Iran;IASBS, Res Ctr Basic Sci & Modern Technol RBST, Zanjan 4513766731, Iran.
    A mononuclear cobalt complex for water oxidation: new controversies and puzzles2018In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 47, no 46, p. 16668-16673Article in journal (Refereed)
    Abstract [en]

    Herein the role of a mononuclear cobalt(iii) complex, [Co-III(DPKOH)(2)]ClO4 (DPK = di(2-pyridyl)ketone), in the water electrooxidation process is investigated with scanning electron microscopy, energy dispersive spectrometry, X-ray diffraction studies, NMR, chronoamperometry, cyclic voltammetry, extended X-ray absorption fine structure and X-ray absorption near edge structure determination. Our experiments show that, in comparison to the reported literature, other cobalt-containing structures on the surface of the FTO electrode could also be the true catalyst for water oxidation.

  • 53.
    Schwartz, Lennart
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Photochemistry and Molecular Science.
    Eriksson, Lars
    Lomoth, Reiner
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Photochemistry and Molecular Science.
    Ott, Sascha
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Photochemistry and Molecular Science.
    Viñas, Clara
    Teixidor, Francesc
    Influence of an electron-deficient bridging o-carborane on the electronic properties of an [FeFe] hydrogenase active site model2008In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, no 18, p. 2379-2381Article in journal (Refereed)
    Abstract [en]

    The IR carbonyl stretching frequencies of [Fe-2(SRS)(CO)(6)] complexes correlate well with their first reduction potential; an [FeFe] hydrogenase model with a very mild reduction potential has been realized by using a strongly electron deficient carborane-dithiolate bridge.

  • 54. Semenaka, Valentyna V.
    et al.
    Nesterova, Oksana V.
    Kokozay, Volodymyr N.
    Zybatyuk, Roman I.
    Shishkin, Oleg V.
    Boca, Roman
    Shevchenko, Denys V.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Photochemistry and Molecular Science, Molecular Biomimetics.
    Huang, Ping
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Photochemistry and Molecular Science, Molecular Biomimetics.
    Styring, Stenbjörn
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Photochemistry and Molecular Science, Molecular Biomimetics.
    Direct synthesis of an heterometallic {(Mn3Cr4III)-Cr-II} wheel by decomposition of Reineckes salt2010In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 39, no 9, p. 2344-2349Article in journal (Refereed)
    Abstract [en]

    A new heterometallic Mn/Cr molecular wheel complex has been synthesized using zerovalent manganese, Reineckes salt, ammonium thiocyanate and triethanolamine (H(3)tea) as starting materials. The compound [Mn3Cr4(NCS)(6)(Htea)(6)] (1) has been characterized in terms of its electrochemical, IR and EPR spectroscopic as well as its magnetic properties. The magnetic susceptibility and magnetization data were treated simultaneously during the optimization routine and resulted in J(Mn-Cr) = + 0.43 cm(-1), J(Cr-Cr) = -4.75 cm(-1), J(Mn-Mn) = +1.78 cm(-1), g(eff) = 1.878 with the ground state S = 15/2.

  • 55.
    Shatskiy, Andrey
    et al.
    Stockholm Univ, Arrhenius Lab, Dept Organ Chem, S-10691 Stockholm, Sweden..
    Lomoth, Reiner
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Abdel-Magied, Ahmed F.
    Stockholm Univ, Arrhenius Lab, Dept Organ Chem, S-10691 Stockholm, Sweden..
    Rabten, Wangchuk
    Stockholm Univ, Arrhenius Lab, Dept Organ Chem, S-10691 Stockholm, Sweden..
    Laine, Tanja M.
    Stockholm Univ, Arrhenius Lab, Dept Organ Chem, S-10691 Stockholm, Sweden..
    Chen, Hong
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden.;KTH Royal Inst Technol, Dept Chem, S-10044 Stockholm, Sweden..
    Sun, Junliang
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden..
    Andersson, Pher G.
    Stockholm Univ, Arrhenius Lab, Dept Organ Chem, S-10691 Stockholm, Sweden..
    Karkas, Markus D.
    Stockholm Univ, Arrhenius Lab, Dept Organ Chem, S-10691 Stockholm, Sweden..
    Johnston, Eric V.
    Stockholm Univ, Arrhenius Lab, Dept Organ Chem, S-10691 Stockholm, Sweden..
    Akermark, Bjorn
    Stockholm Univ, Arrhenius Lab, Dept Organ Chem, S-10691 Stockholm, Sweden..
    Catalyst solvent interactions in a dinuclear Ru-based water oxidation catalyst2016In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 45, no 47, p. 19024-19033Article in journal (Refereed)
    Abstract [en]

    Photocatalytic water oxidation represents a key process in conversion of solar energy into fuels and can be facilitated by the use of molecular transition metal-based catalysts. A novel straightforward approach for covalent linking of the catalytic units to other moieties is demonstrated by preparation of a dinuclear complex containing two [Ru(pdc)(pic)(3)]-derived units (pdc = 2,6-pyridinedicarboxylate, pic = 4-picoline). The activity of this complex towards chemical and photochemical oxidation of water was evaluated and a detailed insight is given into the interactions between the catalyst and acetonitrile, a common co-solvent employed to increase solubility of water oxidation catalysts. The solvent-induced transformations were studied by electrochemical and spectroscopic techniques and the relevant quantitative parameters were extracted.

  • 56.
    Shevchenko, Denys
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - BMC, Analytical Chemistry.
    Huang, Ping
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Bon, Volodymyr V.
    Anderlund, Magnus F.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Kokozay, Vladimir N.
    Styring, Stenbjörn
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Thapper, Anders
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Synthesis, crystal structure, mass spectrometry, electrochemistry and magnetism of a Mn-III-substituted trilacunary Keggin tungstosilicate2013In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 42, no 14, p. 5130-5139Article in journal (Refereed)
    Abstract [en]

    A rare example of a "monomeric" triple transition-metal substituted Keggin anion has been synthesized and characterized by various methods including X-ray crystallography, ESI and MALDI mass spectrometry, electrochemistry, EPR, and SQUID.

  • 57. Soroka, Inna L.
    et al.
    Tarakina, Nadezda V.
    Hermansson, Anton
    Bigum, Lukas
    Widerberg, Rickard
    Andersson, Mikael
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Mathieu, Roland
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Paulraj, Alagar R.
    Kiros, Yohannes
    Radiation-induced synthesis of nanoscale Co-and Ni-based electro-catalysts on carbon for the oxygen reduction reaction2017In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 46, no 30, p. 9995-10002Article in journal (Refereed)
    Abstract [en]

    A facile synthesis of 3d-metal based electro-catalysts directly incorporated into a carbon support was carried out by.-radiation. Transition metals of period 4, i.e. Ni and Co, were precipitated and reduced from their respective salt solutions. The obtained materials were characterized by XRD, SEM, SQUID and the BET methods. Thereafter, the electrodes for fuel cells were fabricated out of synthesized material and their electrochemical performance for the oxygen reduction reaction in 6 M KOH was measured. Although the concentrations of Co and Ni in the electrode material were low (3.4% Co and 0.4% Ni) after reduction by irradiation, both the Ni and Co-based gas diffusion electrodes showed high catalytic activity for oxygen reduction both at room temperature and at 60 degrees C.

  • 58.
    Sundaram, Manickam Minakshi
    et al.
    Murdoch Univ, Dept Chem, Murdoch, WA 6150, Australia..
    Watcharatharapong, Teeraphat
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
    Chakraborty, Sudip
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
    Ahuja, Rajeev
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
    Duraisamy, Shanmughasundaram
    Indian Inst Sci, Inorgan & Phys Chem, Bangalore 560012, Karnataka, India..
    Rao, Penki Tirupathi
    Indian Inst Sci, Inorgan & Phys Chem, Bangalore 560012, Karnataka, India..
    Munichandraiah, Nookala
    Indian Inst Sci, Inorgan & Phys Chem, Bangalore 560012, Karnataka, India..
    Synthesis, and crystal and electronic structure of sodium metal phosphate for use as a hybrid capacitor in non-aqueous electrolyte2015In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 44, no 46, p. 20108-20120Article in journal (Refereed)
    Abstract [en]

    Energy storage devices based on sodium have been considered as an alternative to traditional lithium based systems because of the natural abundance, cost effectiveness and low environmental impact of sodium. Their synthesis, and crystal and electronic properties have been discussed, because of the importance of electronic conductivity in supercapacitors for high rate applications. The density of states of a mixed sodium transition metal phosphate (maricite, NaMn1/3Co1/3Ni1/3PO4) has been determined with the ab initio generalized gradient approximation (GGA)+Hubbard term (U) method. The computed results for the mixed maricite are compared with the band gap of the parent NaFePO4 and the electrochemical experimental results are in good agreement. A mixed sodium transition metal phosphate served as an active electrode material for a hybrid supercapacitor. The hybrid device (maricite versus carbon) in a nonaqueous electrolyte shows redox peaks in the cyclic voltammograms and asymmetric profiles in the charge-discharge curves while exhibiting a specific capacitance of 40 F g(-1) and these processes are found to be quasi-reversible. After long term cycling, the device exhibits excellent capacity retention (95%) and coulombic efficiency (92%). The presence of carbon and the nanocomposite morphology, identified through X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) studies, ensures the high rate capability while offering possibilities to develop new cathode materials for sodium hybrid devices.

  • 59.
    Szijjarto, Csongor
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - BMC, Physical Organic Chemistry.
    Pershagen, Elias
    Borbas, K. Eszter
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - BMC, Physical Organic Chemistry.
    Functionalisation of lanthanide complexes via microwave-enhanced Cu(I)-catalysed azide-alkyne cycloaddition2012In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 41, no 25, p. 7660-7669Article in journal (Refereed)
    Abstract [en]

    Cu-I-catalysed azide-alkyne cycloaddition reactions were used to functionalise lanthanide(III)-complexes (Ln; La, Eu and Tb) incorporating alkyne or azide reactive groups. Microwave irradiation significantly accelerated the reactions, enabling full conversion to the triazole products in some cases in 5 min. Alkyl and aryl azides and alkyl and aryl alkynes could all serve as coupling partners. These reaction conditions proved efficient for cyclen-tricarboxylates and previously unreactive cyclen-tris-primary amide chelates. The synthesis of heterobimetallic (Eu/Tb, EuTb17 and Eu/La, EuLa17) and heterotrimetallic (Eu/La/Eu) complexes was achieved in up to 60% isolated yield starting from coumarin 2-appended alkynyl complexes Tb16 or La16 and an azido-Eu complex Eu4, and bis-alkynyl La-complex La5 and Eu4, respectively. EuTb17 displayed dual Eu-III and Tb-III-emission upon antenna-centred excitation.

  • 60.
    Tchaplyguine, Maxim
    et al.
    Lund Univ, MAX Lab, POB 118, S-22100 Lund, Sweden.
    Zhang, Chaofan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and Condensed Matter Physics.
    Andersson, Tomas
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and Condensed Matter Physics.
    Björneholm, Olle
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and Condensed Matter Physics.
    Ag-Cu oxide nanoparticles with high oxidation states: towards new high T-c materials2018In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 47, no 46, p. 16660-16667Article in journal (Refereed)
    Abstract [en]

    In Ag-Cu oxides possible to fabricate so far, superconductivity has not been detected, but high conductivity was. In the quest for superconductivity the demand is to create a high and peculiar copper-oxygen coordination. Such coordination makes it non-trivial to determine Cu oxidation states, which may be several and co-existing. Another reason for uncertainty is in oxygen deficiency typical for superconducting crystals. Finally, Cu oxidation is influenced by the other metals in the substance. For chemical fabrication the difficulty is to tune the relative abundances of elements in a fine way. Ag-Cu oxides have been also produced by reactive co-sputtering of Cu and Ag, but the composition with high Cu oxidation states necessary for high conductivity has not been realized. In the present work we have fabricated Ag-Cu-oxide nanoparticles containing Cu and Ag in high oxidation states actual for superconductivity. The fabrication includes reactive sputtering of Ag and Cu metals, their vapour oxidation and aggregation into nanoparticles. The ability to create different and high oxidation states, also co-existing, is demonstrated. The fabrication approach also allows overcoming the poor miscibility of Cu and Ag. The nanoparticle composition and the oxidation states could be determined due to an experimental arrangement in which photoelectron spectroscopy is applied to free nanoparticles in a beam in vacuum, what allows avoiding any contact of the particles to a substrate or atmosphere. The combination of the fabrication and characterization methods has proven to be a powerful approach when fine composition tuning and control are desirable.

  • 61.
    Terebilenko, Kateryna V.
    et al.
    Taras Shevchenko Natl Univ Kiev, Dept Chem, Volodymyrska St 64-13, UA-01601 Kiev, Ukraine..
    Bychkov, Konstantin L.
    Taras Shevchenko Natl Univ Kiev, Dept Chem, Volodymyrska St 64-13, UA-01601 Kiev, Ukraine..
    Baumer, Vyacheslav N.
    STC Inst Single Crystals NAS Ukraine, 60 Lenina Ave, UA-61001 Kharkov, Ukraine..
    Slobodyanik, Nikolay S.
    Taras Shevchenko Natl Univ Kiev, Dept Chem, Volodymyrska St 64-13, UA-01601 Kiev, Ukraine..
    Pavliuk, Mariia V.
    Taras Shevchenko Natl Univ Kiev, Dept Chem, Volodymyrska St 64-13, UA-01601 Kiev, Ukraine.;Natl OO Bogomoletz Med Univ, 13 T Shevchenko Blvd, UA-01601 Kiev, Ukraine..
    Thapper, Anders
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Tokmenko, Inna I.
    Nasieka, Iurii M.
    NAS Sci Ukraine, Lab Opt Submicron Spect, V Lashkarev Inst Semicond Phys, 45 Prosp Nauki Str, UA-03028 Kiev, Ukraine..
    Strelchuk, Viktor V.
    NAS Sci Ukraine, Lab Opt Submicron Spect, V Lashkarev Inst Semicond Phys, 45 Prosp Nauki Str, UA-03028 Kiev, Ukraine..
    Structural transformation of Bi1-x/3V1-xMoxO4 solid solutions for light-driven water oxidationt2016In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 45, no 9, p. 3895-3904Article in journal (Refereed)
    Abstract [en]

    The influence of molybdenum content in the solid solutions of Bi1-x/V-3(1-x),MoxO4 (x = 0.05-0.20) on the morphology, band gap, structure and light -driven water oxidation properties has been studied by scanning electron microscopy, X-ray powder diffraction and vibrational spectroscopy (Raman and infrared). To find out the peculiarities of structural changes for bismuth scheelite-related oxides containing both vanadium and molybdenum crystals of Bi0.98V0.93M0.07O4 have been grown from a K-Bi V-Mo-high-temperature melt and characterized by single crystal X-ray diffraction. For the scheelite-related framework both V and Mo were found to occupy the same positions lowering the point group symmetry of tetrahedra from 4/m to 2/m giving monoclinic distortion for solid solutions with x = 0.05----0.10. The most promising photocatalytic performance was obtained for Bi0.96Mo0.1V0.5004, in which the oxygen evolution could reach 21 mu M in 50 s under visible light of LEDs, lambda = 470 +/- 10 nm, and 820.E cm(-2) s(-1). The changes in catalytic properties are shown to be governed by a crystal structure strain with a maximum obtained for the boundary sample between the monoclinic and tetragonal phase.

  • 62.
    Verendel, Johan
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Biochemistry and Organic Chemistry.
    Andersson, Pher G.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Biochemistry and Organic Chemistry.
    Development of pinene-derived N,P ligands and their utility in catalytic asymmetric hydrogenation2007In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, no 47, p. 5603-5610Article in journal (Refereed)
    Abstract [en]

    New diastereomeric N,P-ligands, derived from the natural product (+)--pinene, have been synthesized and evaluated in iridium-catalyzed asymmetric hydrogenation. The ligands are tetrahydroquinoline derivatives synthesized directly from commercially available -pinene utilizing resolution or recrystallization to separate diastereomers. In reduction of a range of different trisubstituted alkenes the catalysts express very different activities ranging from no activity to high activity. One of the catalysts gives good ee values for some substrates.

  • 63.
    White, Travis A.
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Maji, Somnath
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Ott, Sascha
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Mechanistic insights into electrocatalytic CO2 reduction within [Ru-II(tpy)(NN)X](n+) architectures2014In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 43, no 40, p. 15028-15037Article in journal (Refereed)
    Abstract [en]

    A series of Ru-II-polypyridyl complexes of the design [Ru-II(tpy)(NN)X](n+) (tpy = 2,2':6',2 ''-terpyridine; NN = bidentate polypyridine; X = Cl or CH3CN; n = 1 or 2) have been synthesized and analyzed for their ability to function as electrocatalysts in the reduction of CO2 to CO. Varying the electron-donating/withdrawing character of the NN polypyridyl ligand has allowed for modification of electron density at the formally Ru-II metal center. Complexes where X = Cl- display ligand substitution for CH3CN with differing rates of Cl- dissociation (k(-Cl)), therefore providing a degree of insight into the electron density and thus the chemical activity at the Ru-II center. Detailed analysis of the cyclic voltammograms under argon vs. CO2 atmospheres using multiple switching potentials and scan rates ranging from v = 25-2000 mV s(-1) has painted a picture of how monodentate ligand lability due to NN polypyridyl electron-donating character is related to electrocatalytic CO2 reduction activity of Ru-II-polypyridyl complexes. From these studies, multiple mechanistic pathways towards generating the catalytically active [Ru(tpy(-))(NN-)CO2](0) species are proposed and differ via the order of electrochemical and chemical processes.

  • 64.
    Whittle, Thomas A.
    et al.
    Univ Sydney, Sch Chem, Sydney, NSW 2006, Australia..
    Brant, William R.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry. Univ Sydney, Sch Chem, Sydney, NSW 2006, Australia..
    Hester, James R.
    Australian Nucl Sci & Technol Org, Kirrawee DC, NSW 2253, Australia..
    Gu, Qinfen
    Australian Synchrotron, 800 Blackburn Rd, Clayton, Vic 3168, Australia..
    Schmid, Siegbert
    Univ Sydney, Sch Chem, Sydney, NSW 2006, Australia..
    Tailoring phase transition temperatures in perovskites via A-site vacancy generation2017In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 46, no 22, p. 7253-7260Article in journal (Refereed)
    Abstract [en]

    The structures across the Sr0.8Ti0.6-xZrxNb0.4O3, 0 <= x <= 0.6, defect perovskite series were investigated using complementary synchrotron X-ray and neutron powder diffraction data. The locations of second order compositional and temperature dependent phase transitions between the high symmetry cubic Pm (3) over barm phase and the lower symmetry tetragonal I4/mcm phase were determined. Deviation of the oxygen x coordinate from the high symmetry value and the B-O-B bond angle from 180 degrees as well as the tetragonal strain squared were each found to be suitable order parameters to monitor the transitions. Tolerance factor calculations confirmed that these A-site deficient perovskites retain a higher symmetry to a lower value than their fully occupied counterparts. Therefore, adjusting vacancy concentrations can be employed as a general strategy to design compounds with specifically tailored phase transition temperatures.

  • 65.
    Xiong, Ruisheng
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Andres, Julien
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - BMC.
    Scheffler, Kira
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - BMC.
    Borbas, Eszter
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Synthesis and characterisation of lanthanide-hydroporphyrin dyads2015In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 44, p. 2541-2553Article in journal (Refereed)
    Abstract [en]

    Fluorescence spectroscopy is in many ways the ideal tool for the interrogation of complex biological systems, as it is non-invasive, sensitive, and offers high spatiotemporal resolution. For biomedical imaging luminescent probes absorbing and emitting in the red-to-near infrared (NIR) region are best suited to maximise tissue penetration and minimise damage to cellular components. NIR-emitting lanthanides (Ln) sensitised with red-absorbing antennae are promising candidates for these applications, assuming the challenges of poor photophysical properties and tedious syntheses of the complexes are overcome. Chlorins are porphyrin-type tetrapyrroles with intense red absorption. Recently chlorins have been shown to sensitise Yb and Nd emission when incorporated into Ln-complexes. Here we expand on our previous work, and explore the effect of chlorin structure, metallation state, chlorin-Ln-complex linker length and mode of attachment on the properties of chlorin-Ln complexes. As chlorin absorption bands are approximately 20 nm fwhm and readily tunable, a deeper understanding of structure-property relationships would enable the use of chlorin-Ln complexes in multicolour imaging using antenna-specific excitation. A detailed description of antenna and complex syntheses and photophysical characterisation is given. A number of challenges were identified, which will have to be addressed in future studies to enable multicolour imaging using the NIR-emitting lanthanides.

  • 66.
    Xiong, Ruisheng
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - BMC, Physical Organic Chemistry.
    Andres, Julien
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - BMC, Physical Organic Chemistry.
    Scheffler, Kira
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - BMC, Physical Organic Chemistry.
    Borbas, Eszter K.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - BMC, Physical Organic Chemistry.
    Synthesis and characterisation of lanthanide-hydroporphyrin dyads2015In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 44, no 6, p. 2541-2553Article in journal (Refereed)
    Abstract [en]

    Fluorescence spectroscopy is in many ways the ideal tool for the interrogation of complex biological systems, as it is non-invasive, sensitive, and offers high spatiotemporal resolution. For biomedical imaging luminescent probes absorbing and emitting in the red-to-near infrared (NIR) region are best suited to maximise tissue penetration and minimise damage to cellular components. NIR-emitting lanthanides (Ln) sensitised with red-absorbing antennae are promising candidates for these applications, assuming the challenges of poor photophysical properties and tedious syntheses of the complexes are overcome. Chlorins are porphyrin-type tetrapyrroles with intense red absorption. Recently chlorins have been shown to sensitise Yb and Nd emission when incorporated into Ln-complexes. Here we expand on our previous work, and explore the effect of chlorin structure, metallation state, chlorin-Ln-complex linker length and mode of attachment on the properties of chlorin-Ln complexes. As chlorin absorption bands are similar to 20 nm fwhm and readily tunable, a deeper understanding of structure-property relationships would enable the use of chlorin-Ln complexes in multicolour imaging using antenna-specific excitation. A detailed description of antenna and complex syntheses and photophysical characterisation is given. A number of challenges were identified, which will have to be addressed in future studies to enable multicolour imaging using the NIR-emitting lanthanides.

  • 67.
    Xu, Chao
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Sheng, Ming-Ming
    Shi, Hua-Tian
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Zhang, Qian-Feng
    Interlinking supertetrahedral chalcogenolate clusters with bipyridines to form two-dimensional coordination polymers for photocatalytic degradation of organic dye2019In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 48, p. 5505-5510Article in journal (Refereed)
    Abstract [en]

    Chalcogenolate clusters Cd6Ag4(EPh)16(DMF)3(CH3OH) (E = S, Se) with supertetrahedral structures are isolated. Further interlinking the clusters with organic linker 4,4′-trimethylenedipiperidine in the stepwise assembly approach forms two-dimensional coordination polymers. The clusters and the coordination polymers show tunable band gaps and efficient photocatalytic activities for the degradation of aqueous dye solution. This study demonstrates the great potential of using chalcogenolate clusters and their coordination polymers in photocatalysis applications.

  • 68. Yu, Ze
    et al.
    Vlachopoulos, Nick
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Physical and Analytical Chemistry, Physical Chemistry.
    Gorlov, Mikhail
    Kloo, Lars
    Liquid electrolytes for dye-sensitized solar cells2011In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 40, no 40, p. 10289-10303Article in journal (Refereed)
    Abstract [en]

    The present review offers a survey of liquid electrolytes used in dye-sensitized solar cells from the beginning of photoelectrochemical cell research. It handles both the solvents employed, and the prerequisites identified for an ideal liquid solvent, as well as the various effects of electrolyte solutes in terms of redox systems and additives. The conclusions of the present review call for more detailed molecular insight into the electrolyte-electrode interface reactions and structures.

  • 69.
    Zhao, Jie
    et al.
    NW Univ Xian, Coll Chem & Mat Sci, Minist Educ, Key Lab Synthet & Nat Funct Mol Chem, Xian 710069, Peoples R China..
    Yang, Dong
    NW Univ Xian, Coll Chem & Mat Sci, Minist Educ, Key Lab Synthet & Nat Funct Mol Chem, Xian 710069, Peoples R China..
    Zhao, Yanxia
    NW Univ Xian, Coll Chem & Mat Sci, Minist Educ, Key Lab Synthet & Nat Funct Mol Chem, Xian 710069, Peoples R China..
    Cao, Liping
    NW Univ Xian, Coll Chem & Mat Sci, Minist Educ, Key Lab Synthet & Nat Funct Mol Chem, Xian 710069, Peoples R China..
    Zhang, Zhibin
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
    Yang, Xiao-Juan
    NW Univ Xian, Coll Chem & Mat Sci, Minist Educ, Key Lab Synthet & Nat Funct Mol Chem, Xian 710069, Peoples R China..
    Wu, Biao
    NW Univ Xian, Coll Chem & Mat Sci, Minist Educ, Key Lab Synthet & Nat Funct Mol Chem, Xian 710069, Peoples R China..
    Phosphate-induced fluorescence of a tetraphenylethene-substituted tripodal tris(urea) receptor2016In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 45, no 17, p. 7360-7365Article in journal (Refereed)
    Abstract [en]

    A tetraphenylethene (TPE)-decorated tripodal tris(urea) ligand L was synthesized, which shows large emission enhancement when binding to an orthophosphate anion (PO43-), but exhibits only weak or no fluorescence with other anions. The anion-binding and fluorescence properties were studied by X-ray crystal structure, NMR and fluorescence spectroscopy, and by DFT computations and the results demonstrate that the different fluorescence performance may be determined by the anion-binding modes (i.e., full-or half-encapsulation).

  • 70. Zienkiewicz, Małgorzata
    et al.
    Szlachetko, Jakub
    Lothschütz, Christian
    Hodorowicz, Maciej
    Jabłońska-Wawrzycka, Agnieszka
    Sá, Jacinto
    Barszcz, Barbara
    A novel single-site manganese(II) complex of a pyridine derivative as a catalase mimetic for disproportionation of H2O2 in water.2013In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 42, no 21, p. 7761-7Article in journal (Refereed)
    Abstract [en]

    A novel single site Mn(II) complex was successfully synthesized and tested in the aqueous disproportionation of hydrogen peroxide. The complex was found to be stable (HR-XAS) and exhibits catalase-like activity in neutral pH. Theoretical calculations suggested a reaction mechanism involving two complexes, changes in metal oxidation state and proton shuttling.

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