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  • 1.
    Duan, Lele
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Tong, L.
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Towards the Visible Light-Driven Water Splitting Device: Ruthenium Water Oxidation Catalysts with Carboxylate-Containing Ligands2014In: Molecular Water Oxidation Catalysis: A Key Topic for New Sustainable Energy Conversion Schemes, Wiley-Blackwell, 2014, p. 51-76Chapter in book (Other academic)
    Abstract [en]

    The presence of oxo and carboxylate ligands is crucial to decreasing the redox potentials of the oxygen evolving complex (OEC). It has been proved that negatively charged ligands can stabilize the high oxidation states of various transition metal-based complexes and lower their oxidation potentials. This chapter focuses on complexation of transition metals primarily ruthenium (Ru) with carboxylate-containing ligands, in order to develop artificial water oxidation catalysts (WOCs) with small overpotentials. The authors aim at applying highly active and robust WOCs in artificial photosynthesis devices that convert photo energy to chemical energy. A typical visible light-driven water oxidation system consists of three components: a WOC, a photosensitizer, and a sacrificial electron acceptor. The chapter demonstrates a density functional theory (DFT)-directed development of robust Ru-WOCs, showing one of the advantages of molecular WOCs.

  • 2.
    Duan, Lele
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Tong, Lianpeng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Xu, Yunhua
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Visible light-driven water oxidation-from molecular catalysts to photoelectrochemical cells2011In: Energy & Environmental Science, ISSN 1754-5692, E-ISSN 1754-5706, Vol. 4, no 9, p. 3296-3313Article in journal (Refereed)
    Abstract [en]

    This perspective article reports the most significant advances in the field of water oxidation-from molecular water oxidation catalysts (WOCs) to photoelectrochemical cells. Different series of catalysts that can be applied in visible light-driven water oxidation catalysis are discussed in details and several key aspects of their catalytic mechanisms are introduced. In order to construct a water oxidation electrode from molecular catalysts, proper immobilization methods have to be employed. Herein, we present one section about how to attach catalysts onto an electrode/material surface. Finally, the state of the art photoelectrochemical cells that achieve visible light-driven water splitting are described.

  • 3.
    Duan, Lele
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Xu, Yunhua
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Gorlov, Mikhail
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Tong, Lianpeng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Andersson, Samir
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Chemical and Photochemical Water Oxidation Catalyzed by Mononuclear Ruthenium Complexes with a Negatively Charged Tridentate Ligand2010In: Chemistry - A European Journal, ISSN 0947-6539, E-ISSN 1521-3765, Vol. 16, no 15, p. 4659-4668Article in journal (Refereed)
    Abstract [en]

    Two mononuclear ruthenium complexes [RuL(pic)(3)] (1) and [RuL(bpy)(pic)] (2) (H2L = 2,6-pyridinedicarboxylic acid, pic=4-picoline, bpy = 2,2'-bipyridine) have been synthesized and fully characterized. Both complexes could promote water oxidation chemically and photochemically. Compared with other known ruthenium-based water oxidation catalysts using [Ce(NH4)(2)(NO3)(6)] (Ce-IV) as the oxidant in solution at pH 1.0, complex 1 is one of the most active catalysts yet reported with an initial rate of 0.23 turnovers(-1). Under acidic conditions, the equatorial 4-picoline in complex 1 dissociates first. In addition, ligand exchange in 1 occurs when the Rum state is reached. Based on the above observations and MS measurements of the intermediates during water oxidation by 1 using Ce-IV as oxidant, [RuL(pic)(2)(H2O)](+) is proposed as the real water oxidation catalyst.

  • 4.
    Duan, Lele
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Xu, Yunhua
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Tong, Lianpeng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Ce-IV- and Light-Driven Water Oxidation by [Ru(terpy)(pic)(3)](2+) Analogues: Catalytic and Mechanistic Studies2011In: CHEMSUSCHEM, ISSN 1864-5631, Vol. 4, no 2, p. 238-244Article in journal (Refereed)
    Abstract [en]

    A series of mononuclear ruthenium polypyridyl complexes [Ru(Mebimpy)(pic)(3)](PF6)(2) (2; Mebimpy=2,6-bis(1-methylbenzimidazol-2-yl)pyridine; pic=4-picoline), Ru(bimpy)(pic)(3) (3; H(2)bimpy=2,6-bis(benzimidazol-2-yl)pyridine), trans-[Ru(terpy)-(pic)(2)Cl](PF6) (4; terpy=2,2';6',2 ''-terpyridine), and trans-[Ru(terpy)(pic)(2)(OH2)](ClO4)(2) (5) are synthesized and characterized as analogues of the known Ru complex, [Ru(terpy)(pic)(3)](PF6)(2) (1). The effect of the ligands on electronic and catalytic properties is studied and discussed. The negatively charged ligand, bimpy(2-), has a remarkable influence on the electrochemical events due to its strong electron-donating ability. The performance in light- and Ce-IV-driven (Ce-IV=Ce(NH4)(2)(NO3)(6)) water oxidation is successfully demonstrated. We propose that ligand exchange between pic and H2O occurs to form the real catalyst, a Ru-aqua complex. The synthesis and testing of trans[Ru(terpy)(pic)(2)(OH2)](ClO4)(2) (5) confirmed our proposal. In addition, complex 5 possesses the best catalytic activity among these five complexes.

  • 5.
    Li, Fusheng
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry.
    Li, Lin
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Tong, Lianpeng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Daniel, Quentin
    KTH, School of Chemical Science and Engineering (CHE), Chemistry.
    Göthelid, Mats
    KTH, School of Information and Communication Technology (ICT), Materials- and Nano Physics, Material Physics, MF.
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry. KTH, School of Chemical Science and Engineering (CHE), Centres, Centre of Molecular Devices, CMD.
    Immobilization of a molecular catalyst on carbon nanotubes for highly efficient electro-catalytic water oxidation2014In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 50, no 90, p. 13948-13951Article in journal (Refereed)
    Abstract [en]

    Electrochemically driven water oxidation has been performed using a molecular water oxidation catalyst immobilized on hybrid carbon nanotubes and nano-material electrodes. A high turnover frequency (TOF) of 7.6 s(-1) together with a high catalytic current density of 2.2 mA cm(-2) was successfully obtained at an overpotential of 480 mV after 1 h of bulk electrolysis.

  • 6.
    Staehle, Robert
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry.
    Tong, Lianpeng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Wang, Lei
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Duan, Lele
    KTH, School of Chemical Science and Engineering (CHE), Chemistry.
    Fischer, Andreas
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Ahlquist, Mårten S. G.
    KTH, School of Biotechnology (BIO), Theoretical Chemistry and Biology.
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Rau, Sven
    Water oxidation catalyzed by mononuclear ruthenium complexes with a 2,2′-bipyridine-6,6′-dicarboxylate (bda) ligand: How ligand environment influences the catalytic behavior2014In: Inorganic Chemistry, ISSN 0020-1669, E-ISSN 1520-510X, Vol. 53, no 3, p. 1307-1319Article in journal (Refereed)
    Abstract [en]

    A new water oxidation catalyst [RuIII(bda)(mmi)(OH 2)](CF3SO3) (2, H2bda = 2,2′-bipyridine-6,6′-dicarboxylic acid; mmi = 1,3- dimethylimidazolium-2-ylidene) containing an axial N-heterocyclic carbene ligand and one aqua ligand was synthesized and fully characterized. The kinetics of catalytic water oxidation by 2 were measured using stopped-flow technique, and key intermediates in the catalytic cycle were probed by density functional theory calculations. While analogous Ru-bda water oxidation catalysts [Ru(bda)L2] (L = pyridyl ligands) are supposed to catalyze water oxidation through a bimolecular coupling pathway, our study points out that 2, surprisingly, undergoes a single-site water nucleophilic attack (acid-base) pathway. The diversion of catalytic mechanisms is mainly ascribed to the different ligand environments, from nonaqua ligands to an aqua ligand. Findings in this work provide some critical proof for our previous hypothesis about how alternation of ancillary ligands of water oxidation catalysts influences their catalytic efficiency.

  • 7.
    Tong, Lianpeng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Mononuclear Ruthenium Complexes that Catalyze Water to Dioxgen Oxidation2012Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    The theme of this thesis is the development of mononuclear Ru-based complexes that are capable of catalyzing the water oxidation (or O2-evolving) reaction, e.g. 2 H2O → O2 + 4 H+ + 4 e. Several families of mononuclear Ru water oxidation catalysts were designed and prepared. They feature with anionic ancillary ligands that contain carboxylate or phenolate donors. The properties of the catalysts were investigated in various aspects including coordination geometry, electrochemical behavior, and ligand exchange. All catalysts showed outstanding catalytic activity towards water oxidation in the presence of cerium(IV) ammonium nitrate as a sacrificial oxidant. High-valent Ru intermediates involved in the reactions were characterized both experimentally and theoretically. The kinetics of catalytic water oxidation was examined based on one catalyst and a prevailing catalytic pathway was proposed. The catalytic cycle involved a sequence of oxidation steps from RuII−OH2 to RuV=O species and O−O bond formation via water-nucleophilic-attack to the RuV=O intermediate. By comparing properties and catalytic performance of Ru catalysts herein with that of previously reported examples, the effect of anionic ancillary ligands was clearly elucidated in the context of catalytic water oxidation. Aiming to further application in an envisaged artificial photosynthesis device, visible light-driven water oxidation was conducted and achieved primarily in a homogeneous three-component system containing catalyst, photosensitizer, and sacrificial electron acceptor. Moreover, one model Ru catalyst was successfully immobilized on ordinary glass carbon surface through a facile and widely applicable method.

  • 8.
    Tong, Lianpeng
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Duan, Lele
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Xu, Yunhua
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Privalov, Timofei
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry. KTH, School of Chemical Science and Engineering (CHE), Centres, Centre of Molecular Devices, CMD.
    Structural Modifications of Mononuclear Ruthenium Complexes: A Combined Experimental and Theoretical Study on the Kinetics of Ruthenium-Catalyzed Water Oxidation2011In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 50, no 2, p. 445-449Article in journal (Refereed)
    Abstract [en]

    Small change, big difference: A minor structural modification of water-oxidation catalysts changes the kinetics of O2 evolution from second- to first-order (see scheme). According to DFT calculations, the torsional flexibility of the chelating ligands and their reorganization through the catalytic cycle are implicated in pathway selectivity, and the auxiliary carboxylate group becomes involved in proton-coupled nucleophilic attack.

  • 9.
    Tong, Lianpeng
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Götelid, Mats
    KTH, School of Information and Communication Technology (ICT), Microelectronics and Applied Physics, MAP.
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Oxygen evolution at functionalized carbon surfaces: A strategy for immobilization of molecular water oxidation catalysts2012In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 48, no 80, p. 10025-10027Article in journal (Refereed)
    Abstract [en]

    A molecular Ru(ii) water oxidation catalyst was immobilized on a conductive carbon surface through a covalent bond, and its activity was maintained at the same time. The method can be applied to other materials and may inspire development of artificial photosynthesis devices.

  • 10.
    Tong, Lianpeng
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Inge, A. Ken
    Stockholm University.
    Duan, Lele
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Wang, Lei
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Zou, Xiaodong
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Catalytic Water Oxidation by Mononuclear Ru Complexes with an Anionic Ancillary Ligand2013In: Inorganic Chemistry, ISSN 0020-1669, E-ISSN 1520-510X, Vol. 52, no 5, p. 2505-2518Article in journal (Refereed)
    Abstract [en]

    Mononuclear Ru-based water oxidation catalysts containing anionic ancillary ligands have shown promising catalytic efficiency and intriguing properties. However, their insolubility in water restricts a detailed mechanism investigation. In order to overcome this disadvantage, complexes [Ru-II(bpc)(bpy)OH2](+) (1(+), bpc = 2,2'-bipyridine-6-carboxylate, bpy = 2,2'-bipyridine) and [Ru-II(bpc)(pic)(3)](+) (2(+), pic = 4-picoline) were prepared and fully characterized, which features an anionic tridentate ligand and has enough solubility for spectroscopic study in water. Using Ce-IV as an electron acceptor, both complexes are able to catalyze O-2-evolving reaction with an impressive rate constant. On the basis of the electrochemical and kinetic studies, a water nucleophilic attack pathway was proposed as the dominant catalytic cycle of the catalytic water oxidation by 1(+), within which several intermediates were detected by MS. Meanwhile, an auxiliary pathway that is related to the concentration of Ce-IV was also revealed. The effect of anionic ligand regarding catalytic water oxidation was discussed explicitly in comparison with previously reported mononuclear Ru catalysts carrying neutral tridentate ligands, for example, 2,2':6',2 ''-terpyridine (tpy). When 2(+) was oxidized to the trivalent state, one of its picoline ligands dissociated from the Ru center. The rate constant of picoline dissociation was evaluated from time-resolved UV-vis spectra.

  • 11.
    Tong, Lianpeng
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry.
    Wang, Ying
    KTH, School of Biotechnology (BIO), Theoretical Chemistry and Biology.
    Duan, Lele
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Xu, Yunhua
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Cheng, Xiao
    KTH, School of Biotechnology (BIO), Theoretical Chemistry and Biology.
    Fischer, Andreas
    KTH, School of Chemical Science and Engineering (CHE), Chemistry.
    Ahlquist, Mårten S. G.
    KTH, School of Biotechnology (BIO), Theoretical Chemistry and Biology.
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Water Oxidation Catalysis: Influence of Anionic Ligands upon the Redox Properties and Catalytic Performance of Mononuclear Ruthenium Complexes2012In: Inorganic Chemistry, ISSN 0020-1669, E-ISSN 1520-510X, Vol. 51, no 6, p. 3388-3398Article in journal (Refereed)
    Abstract [en]

    Aiming at highly efficient molecular catalyts for water oxidation, a mononuclear ruthenium complex Ru-II(hqc)(pic)(3) (1; H(2)hqc = 8-hydroxyquinoline-2-carboxylic acid and plc = 4-picoline) containing negatively charged carboxylate and phenolate donor groups has been designed and synthesized. As a comparison, two reference complexes, Ru-II(pdc)(pic)(3) (2; H(2)pdc = 2,6-pyridine-dicarboxylic acid) and Ru-II(tpy)(pic)(3) (3; tpy = 2,2':6',2 ''-terpyridine), have also been prepared. All three complexes are fully characterized by NMR, mass spectrometry (MS), and X-ray crystallography. Complex 1 showed a high efficiency toward catalytic water oxidation either driven by chemical oxidant (Ce-IV in a pH 1 solution) with a initial turnover number of 0.32 s(-1), which is several orders of magnitude higher than that of related mononuclear ruthenium catalysts reported in the literature, or driven by visible light in a three-component system with [Ru(bpy)(3)](2+) types of photosensitizers. Electrospray ionization MS results revealed that at the Rum state complex 1 undergoes ligand exchange of 4-picoline with water, forming the authentic water oxidation catalyst in situ. Density functional theory (DFT) was ernployed to explain how anionic ligands (hqc and pdc) facilitate the 4-picoline dissociation compared with a neutral ligand (tpy). Electrochemical measurements show that complex 1 has a much lower E(Ru-III/Ru-II) than that of reference complex 2 because of the introduction of a phenolate ligand. DFT was further used to study the influence of anionic ligands upon the redox properties of mononuclear aquaruthenium species, which are postulated to be involved in the catalysis cycle of water oxidation.

  • 12.
    Wang, Lei
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry.
    Duan, Lele
    KTH, School of Chemical Science and Engineering (CHE), Chemistry.
    Tong, Lianpeng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry.
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Visible light-driven water oxidation catalyzed by mononuclear ruthenium complexes2013In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 306, p. 129-132Article in journal (Refereed)
    Abstract [en]

    A series of mononuclear ruthenium water oxidation catalysts (WOCs) [Ru(bda)L-2] (H(2)bda = 2,2'-bipyridine-6,6'-dicarboxylic acid; L = N-cyclic aromatic ligands) were investigated in three-component light-driven water oxidation systems composed of photosensitizers, a sacrificial electron acceptor, and WOCs. A high turnover number of 579 for water oxidation was achieved in the homogeneous system using complex 4 ([Ru(bda)(4-Br-pyridine)(2)]) as the WOC, and a high quantum efficiency of 17% was found which is a new record for visible light-driven water oxidation in homogeneous systems.

  • 13.
    Xu, Yunhua
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Duan, Lele
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Akermark, Torbjorn
    Tong, Lianpeng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Lee, Bao-Lin
    Zhang, Rong
    Akermark, Bjorn
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Synthesis and Catalytic Water Oxidation Activities of Ruthenium Complexes Containing Neutral Ligands2011In: Chemistry - A European Journal, ISSN 0947-6539, E-ISSN 1521-3765, Vol. 17, no 34, p. 9520-9528Article in journal (Refereed)
    Abstract [en]

    Two dinuclear and one mononuclear ruthenium complexes containing neutral polypyridyl ligands have been synthesised as pre-water oxidation catalysts and characterised by (1)H and (13)C NMR spectroscopy and ESI-MS. Their catalytic water oxidation properties in the presence of [Ce(NH(4))(2)(NO(3))(6)] (Ce(IV)) as oxidant at pH 1.0 have been investigated. At low concentrations of Ce(IV) (5 mm), high turnover numbers of up to 4500 have been achieved. An (18)O-labelling experiment established that both O atoms in the evolved O(2) originate from water. Combined electrochemical study and electrospray ionisation mass spectrometric analysis suggest that ligand exchange between coordinated 4-picoline and free water produces Ru aquo species as the real water oxidation catalysts.

  • 14.
    Xu, Yunhua
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Duan, Lele
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Tong, Lianpeng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Akermark, Bjorn
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Visible light-driven water oxidation catalyzed by a highly efficient dinuclear ruthenium complex2010In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 46, no 35, p. 6506-6508Article in journal (Refereed)
    Abstract [en]

    Visible light-driven water oxidation has been achieved by the dinuclear ruthenium complex 1 with a high turnover number of 1270 in a homogeneous system in the presence of a Ru polypyridine complex photosensitizer.

  • 15.
    Xu, Yunhua
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Fischer, Andreas
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Inorganic Chemistry.
    Duan, Lele
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Tong, Lianpeng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Gabrielsson, Erik
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Åkermark, Björn
    Sun, Licheng
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
    Chemical and Light-Driven Oxidation of Water Catalyzed by an Efficient Dinuclear Ruthenium Complex2010In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 49, no 47, p. 8934-8937Article in journal (Refereed)
1 - 15 of 15
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