| 1. |
- Duan, Lele, et al.
(författare)
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Ce-IV- and Light-Driven Water Oxidation by [Ru(terpy)(pic)(3)](2+) Analogues : Catalytic and Mechanistic Studies
- 2011
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Ingår i: CHEMSUSCHEM. - : Wiley. - 1864-5631. ; 4:2, s. 238-244
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 2. |
- Duan, Lele, et al.
(författare)
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Chemical and Photochemical Water Oxidation Catalyzed by Mononuclear Ruthenium Complexes with a Negatively Charged Tridentate Ligand
- 2010
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Ingår i: Chemistry - A European Journal. - : Wiley. - 0947-6539 .- 1521-3765. ; 16:15, s. 4659-4668
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 3. |
- Duan, Lele, et al.
(författare)
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Visible Light-Driven Water Oxidation by a Molecular Ruthenium Catalyst in Homogeneous System
- 2010
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Ingår i: Inorganic Chemistry. - : American Chemical Society (ACS). - 0020-1669 .- 1520-510X. ; 49:1, s. 209-215
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Tidskriftsartikel (refereegranskat)abstract
- Discovery of an efficient catalyst bearing low overpotential toward water oxidation is a key step for light-driven water splitting into dioxygen and dihydrogen. A mononuclear ruthenium complex, Ru(II)L(pic)(2) (1) (H2L = 2,2'-bipyridine-6,6'-dicarboxylic acids pic = 4-picoline), was found capable of oxidizing water eletrochemically at a relatively low potential and promoting light-driven water oxidation using a three-component system composed of a photosensitizer, sacrificial electron acceptor, and complex 1. The detailed electrochemical properties of 1 were studied, and the onset potentials of the electrochemically catalytic curves in pH 7.0 and pH 1.0 solutions are 1.0 and 1.5 V, respectively. The low catalytic potential of 1 under neutral conditions allows the use of [Ru(bpy)(3)](2+) and even [Ru(dmbpy)(3)](2+) as a photosensitizer for photochemical water oxidation. Two different sacrificial electron acceptors, [Co(NH3)(5)Cl]Cl-2 and Na2S2O8, were used to generate the oxidized state of ruthenium tris(2,2'-bipyridyl) photosensitizers. In addition, a two-hour photolysis of I in a pH TO phosphate buffer did not lead to obvious degradation, indicating the good photostability of our catalyst. However, under conditions of light-driven water oxidation, the catalyst deactivates quickly. In both solution and the solid state under aerobic conditions, complex 1 gradually decomposed via oxidative degradation of its ligands, and two of the decomposed products, sp(3) C-H bond oxidized Ru complexes, were identified. The capability of oxidizing the sp(3) C-H bond implies the presence of a highly oxidizing Ru species, which might also cause the final degradation of the catalyst.
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| 4. |
- Duan, Lele, et al.
(författare)
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Visible light-driven water oxidation-from molecular catalysts to photoelectrochemical cells
- 2011
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Ingår i: Energy & Environmental Science. - : Royal Society of Chemistry (RSC). - 1754-5692 .- 1754-5706. ; 4:9, s. 3296-3313
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 5. |
- Huang, Jing, et al.
(författare)
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Improved Performance of Colloidal CdSe Quantum Dot-Sensitized Solar Cells by Hybrid Passivation
- 2014
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 6:21, s. 18808-18815
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Tidskriftsartikel (refereegranskat)abstract
- A hybrid passivation strategy is employed to modify the surface of colloidal CdSe quantum dots (QDs) for quantum dot-sensitized solar cells (QDSCs), by using mercaptopropionic acid (MPA) and iodide anions through a ligand exchange reaction in solution. This is found to be an effective way to improve the performance of QDSCs based on colloidal QDs. The results show that MPA can increase the coverage of the QDs on TiO2 electrodes and facilitate the hole extraction from the photoxidized QDs, and simultaneously, that the iodide anions can remedy the surface defects of the CdSe QDs and thus reduce the recombination loss in the device. This hybrid passivation treatment leads to a significant enhancement of the power conversion efficiency of the QDSCs by 41%. Furthermore, an optimal ratio of iodide ions to MPA was determined for favorable hybrid passivation; results show that excessive iodine anions are detrimental to the loading of the QDs. This study demonstrates that the improvement in QDSC performance can be realized by using a combination of different functional ligands to passivate the QDs, and that ligand exchange in solution effective approach to introduce can be an different ligands.
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| 6. |
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| 7. |
- Pettersson, Henrik, et al.
(författare)
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Parallel-connected monolithic dye-sensitised solar modules
- 2010
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Ingår i: Progress in Photovoltaics. - : Wiley. - 1062-7995 .- 1099-159X. ; 18:5, s. 340-345
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Tidskriftsartikel (refereegranskat)abstract
- Light-soaking and high-temperature storage testing of monolithic dye-sensitised solar modules with total area module efficiencies above 5% have been performed. Our experiences from the development of a four-layer monolithic dye-sensitised solar test cell for comparative testing of material components for dye-sensitised solar cells have directed our module development to a novel device design consisting of parallel-connection of individual monolithic cells. The results from the accelerated testing of the modules (total area of 17.0 cm(2)) with four parallel-connected cells (active area of 3.38 cm(2)/cell) are equivalent to those obtained for the monolithic single test cells when using identical device components. The successful transfer from cell to module stability is an important milestone in our ambition to develop a low-cost Photovoltaic (PV) technology. Moreover, our results indicate that intensified research and development to define the procedures for relevant accelerated testing of dye-sensitised solar modules is urgently required.
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| 8. |
- Tian, Haining, et al.
(författare)
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Effect of the chromophores structures on the performance of solid-state dye sensitized solar cells
- 2014
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Ingår i: Nano. - 1793-2920. ; 9:5, s. 1440005-
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Tidskriftsartikel (refereegranskat)abstract
- The er effect of metal-free chromophores on dye-sensitized solar cell performance is investigated. Solid state dye-sensitized solar cells (ssDSCs) using dirfferent molecular sensitizers based on tri-phenylamine (TPA) with thiophene linkers and different alkyl chain in the donor unit have been characterized using impedance spectroscopy (IS). We show that different molecular structures play a fundamental role on solar cell performance, by the effect produced on TiO2 conduction band position and in the recombination rate. Dye structure and its electronic properties are the main factors that control the recombination, the capacitance and the efficiency of the cells. A clear trend between the performance of the cell and the optimization level of the blocking effect of the dye structure has been identified in the solid state solar cells with Spiro-OMeTAD hole conductor.
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| 9. |
- Tian, Haining, et al.
(författare)
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Enhancement of p-Type Dye-Sensitized Solar Cell Performance by Supramolecular Assembly of Electron Donor and Acceptor
- 2014
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Ingår i: Scientific Reports. - : Springer Science and Business Media LLC. - 2045-2322. ; 4, s. 4282-
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Tidskriftsartikel (refereegranskat)abstract
- Supramolecular interactions based on porphyrin and fullerene derivatives were successfully adopted to improve the photovoltaic performance of p-type dye-sensitized solar cells (DSCs). Photoelectron spectroscopy (PES) measurements suggest a change in binding configuration of ZnTCPP after co-sensitization with C60PPy, which could be ascribed to supramolecular interaction between ZnTCPP and C60PPy. The performance of the ZnTCPP/C60PPy-based p-type DSC has been increased by a factor of 4 in comparison with the DSC with the ZnTCPP alone. At 560 nm, the IPCE value of DSCs based on ZnTCPP/C60PPy was a factor of 10 greater than that generated by ZnTCPP-based DSCs. The influence of different electrolytes on charge extraction and electron lifetime was investigated and showed that the enhanced V-oc from the Co2+/(3+)(dtbp)(3)-based device is due to the positive E-F shift of NiO.
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| 10. |
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| 11. |
- Tong, Lianpeng, et al.
(författare)
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Water Oxidation Catalysis : Influence of Anionic Ligands upon the Redox Properties and Catalytic Performance of Mononuclear Ruthenium Complexes
- 2012
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Ingår i: Inorganic Chemistry. - : American Chemical Society (ACS). - 0020-1669 .- 1520-510X. ; 51:6, s. 3388-3398
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 12. |
- Xiong, Dehua, et al.
(författare)
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Enhanced Performance of p-Type Dye-Sensitized Solar Cells Based on Ultrasmall Mg-Doped CuCrO2 Nanocrystals
- 2013
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Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 6:8, s. 1432-1437
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Tidskriftsartikel (refereegranskat)abstract
- Herein, we present ultrasmall delafossite-type Mg-doped CuCrO2 nanocrystals prepared by using hydrothermal synthesis and their first application as photocathodes in efficient p-type dye-sensitized solar cells. The short-circuit current density (J(sc)) is notably increased by approximately 27% owing to the decreased crystallite size and the enhanced optical transmittance associated with Mg doping of the CuCrO2 nanocrystalline sample. An open-circuit voltage (V-oc) of 201mV, J(sc) of 1.51mAcm(-2), fill factor of 0.449, and overall photoconversion efficiency of 0.132% have been achieved with the CuCr0.9Mg0.1O2 dye photocathode sensitized with the P1 dye under optimized conditions. This efficiency is nearly threetimes higher than that of the NiO-based reference device, which is attributed to the largely improved V-oc and J(sc). The augmentation of V-oc and J(sc) can be attributed to the lower valance band position and the faster hole diffusion coefficient of CuCr0.9Mg0.1O2 compared to those of the NiO reference, respectively, which leads to a higher hole collection efficiency.
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| 13. |
- Xu, Bo, et al.
(författare)
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AgTFSI as p-Type Dopant for Efficient and Stable Solid-State Dye-Sensitized and Perovskite Solar Cells
- 2014
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Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 7:12, s. 3252-3256
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Tidskriftsartikel (refereegranskat)abstract
- A silver-based organic salt, silver bis(trifluoromethane-sulfonyl) imide (AgTFSI), was employed as an effective p-type dopant for the triarylamine-based organic hole-transport material Spiro-MeOTAD, which has been successfully applied in solid-state dye-sensitized solar cells (ssDSCs) and perovskite solar cells (PSCs). The power conversion efficiencies (PCEs) of AgTFSI-doped devices improved by 20%, as compared to the device based on the commonly used oxygen doping both for ssDSCs and PSCs. Moreover, the solid-state dye-sensitized devices exposed to AgTFSI as dopant showed considerably better stability than those of oxygen doped, qualifying this p-type dopant as a promising alterative for the preparation of highly efficient as well as stable ssDSCs and PSCs for the future.
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| 14. |
- Xu, Bo, et al.
(författare)
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Carbazole-Based Hole-Transport Materials for Efficient Solid-State Dye-Sensitized Solar Cells and Perovskite Solar Cells
- 2014
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Ingår i: Advanced Materials. - : Wiley-VCH Verlagsgesellschaft. - 0935-9648 .- 1521-4095. ; 26:38, s. 6629-6634
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Tidskriftsartikel (refereegranskat)abstract
- (Graph Presented) Two carbazole-based small molecule hole-transport materials (HTMs) are synthesized and investigated in solid-state dye-sensitized solar cells (ssDSCs) and perovskite solar cells (PSCs). The HTM X51-based devices exhibit high power conversion efficiencies (PCEs) of 6.0% and 9.8% in ssDSCs and PSCs, respectively. These results are superior or comparable to those of 5.5% and 10.2%, respectively, obtained for the analogous cells using the state-of-the-art HTM Spiro-OMeTAD.
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| 15. |
- Xu, Bo, et al.
(författare)
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Efficient solid state dye-sensitized solar cells based on an oligomer hole transport material and an organic dye
- 2013
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Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry (RSC). - 2050-7488 .- 2050-7496 .- 0959-9428 .- 1364-5501. ; 1:46, s. 14467-14470
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Tidskriftsartikel (refereegranskat)abstract
- A low-cost and easily-synthesized organic hole transport material (HTM) X3 bearing triphenylamine units and an organic dye was utilized for solid state dye sensitized solar cells (ssDSCs), which have achieved the power conversion efficiencies of 5.8% and 7.1% under 1 sun and 0.46 sun, respectively, outperforming the ssDSC based on Spiro-OMeTAD 5.4% (1 sun) and 6.4% (0.46 sun).
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| 16. |
- Xu, Xiaobao, et al.
(författare)
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Efficient p-type dye-sensitized solar cells based on disulfide/thiolate electrolytes
- 2013
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Ingår i: Nanoscale. - : Royal Society of Chemistry (RSC). - 2040-3364 .- 2040-3372. ; 5:17, s. 7963-7969
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Tidskriftsartikel (refereegranskat)abstract
- Herein, an organic redox couple 1-methy-1H-tetrazole-5-thiolate (T-) and its disulfide dimer (T-2) redox shuttle, as an electrolyte, is introduced in a p-type dye-sensitized solar cell (DSC) on the basis of an organic dye (P1) sensitizer and nanocrystal CuCrO2 electrode. Using this iodide-free transparent redox electrolyte in conjunction with the sensitized heterojunction, we achieve a high open-circuit voltage of over 300 mV. An optimal efficiency of 0.23% is obtained using a CoS counter electrode and an optimized electrolyte composition under AM 1.5 G 100 mW cm(-2) light illumination which, to the best of our knowledge, represents the highest efficiency that has so far been reported for p-type DSCs using organic redox couples.
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| 17. |
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| 18. |
- Xu, Yunhua, et al.
(författare)
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Synthesis and Catalytic Water Oxidation Activities of Ruthenium Complexes Containing Neutral Ligands
- 2011
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Ingår i: Chemistry - A European Journal. - : Wiley. - 0947-6539 .- 1521-3765. ; 17:34, s. 9520-9528
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 19. |
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| 20. |
- Yang, Lei, et al.
(författare)
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Initial Light Soaking Treatment Enables Hole Transport Material to Outperform Spiro-OMeTAD in Solid-State Dye-Sensitized Solar Cells
- 2013
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Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 135:19, s. 7378-7385
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Tidskriftsartikel (refereegranskat)abstract
- Efficient solid state dye-sensitized solar cells (sDSCs) were obtained using a small hole transport material, MeO-TPD (N,N,N',N'-tetrakis(4-methoxyphenyl)benzidine), after an initial light soaking treatment. It was discovered that the light soaking treatment for the MeO-TPD based solar cells is essential in order to achieve the high efficiency (4.9%), which outperforms spiro-OMeTAD based sDSCs using the same dye and device preparation parameters. A mechanism based on Li+ ion migration is suggested to explain the light soaking effect. It was observed that the electron lifetime for the MeO-TPD based sDSC strongly increases after the light soaking treatment, which explains the higher efficiency. After the initial light soaking treatment the device efficiency remains considerably stable with only 0.2% decrease after around 1 month (unsealed cells stored in dark).
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| 21. |
- Yu, Ze, et al.
(författare)
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Ruthenium sensitizer with a thienylvinylbipyridyl ligand for dye-sensitized solar cells
- 2011
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Ingår i: Dalton Transactions. - : Royal Society of Chemistry. - 1477-9226 .- 1477-9234. ; 40:33, s. 8361-8366
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Tidskriftsartikel (refereegranskat)abstract
- A new ruthenium bipyridyl complex, coded as YX360, incorporating a conjugated thienylvinylbipyridyl ligand, cis-Ru(dtbpy)(dcbpy)(NCS)(2) [dtbpy = 4,4'-di(thienylvinyl)-2,2'-bipyridyl; dcbpy = 4,4'-dicarboxy-2,2'-bipyridyl], has been synthesized and studied as a dye in dye-sensitized solar cells (DSCs). The new dye is compared to its precursor N719, which is one of the best ruthenium-based sensitizers known so far. In the dye YX360 the lowest metal-to-ligand charge-transfer (MLCT) band is red-shifted by 10 nm and the molar extinction coefficient is dramatically increased as compared to N719. The reason can largely be attributed to the introduction of the extended pi-conjugation unit to the ruthenium complex. Correspondingly, the incident photon-to-current conversion efficiency (IPCE) spectra of solar cells containing the dye YX360 show relatively higher values in the plateau region and a wider absorption spectrum relative to those of the dye N719. The effect is most pronounced for thinner TiO(2) films, for which comparable overall conversion efficiencies were obtained. However, as the TiO(2) film thickness is increased, DSCs containing N719 show superior conversion efficiencies. Although YX360 typically renders better short-circuit currents, the open-circuit voltage is suppressed because of larger electron recombination losses at the TiO(2)/dye/electrolyte interface. The results highlight that an extended aromatic ligand system in a sensitizing dye on the one hand improved light absorption, but on the other hand more efficiently loses photoelectrons through a recombination pathway via the dye to the electrolyte.
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| 22. |
- Zhang, Biaobiao, et al.
(författare)
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Electrochemical and Photoelectrochemical Water Oxidation by Supported Cobalt-Oxo Cubanes
- 2014
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Ingår i: ACS Catalysis. - : American Chemical Society (ACS). - 2155-5435. ; 4:3, s. 804-809
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Tidskriftsartikel (refereegranskat)abstract
- Cobalt-oxo cubane clusters were immobilized on a Nafion film-coated fluorine-doped tin oxide (FTO) electrode and an alpha-Fe2O3 photoanode as surface catalysts for water oxidation. The performance of electrochemical water splitting indicated that these earth-abundant metal complexes retain their homogeneous reactivity on the electrode. Furthermore, efficient visible light-driven water oxidation was realized by coupling a molecular electrocatalyst with an inorganic semiconductor as a noble metal-free photoanode, showing a stability significantly improved with respect to that of the homogeneous system.
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| 23. |
- Zhang, Biaobiao, et al.
(författare)
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Homogeneous Oxidation of Water by Iron Complexes with Macrocyclic Ligands
- 2014
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Ingår i: Chemistry - An Asian Journal. - : Wiley. - 1861-4728 .- 1861-471X. ; 9:6, s. 1515-1518
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Tidskriftsartikel (refereegranskat)abstract
- The activity of eleven separated iron complexes and nine in situ-generated iron complexes towards catalytic water oxidation have been examined in aqueous solutions with Ce(NH4)(2)(NO3)(6) as the oxidant. Two iron complexes bearing tridentate and tetradentate macrocyclic ligands were found to be novel water oxidation catalysts. The one with tetradentate ligand exhibited a promising activity with a turnover number of 65 for oxygen evolution.
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| 24. |
- Zhou, Xu, et al.
(författare)
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Photocatalytic Water Oxidation by Molecular Assemblies Based on Cobalt Catalysts
- 2014
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Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 7:9, s. 2453-2456
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Tidskriftsartikel (refereegranskat)abstract
- Chromophore-catalyst molecular assemblies towards visible light-driven water oxidation were synthesized by covalent integration of a light-harvesting complex [Ru(bpy)(3)](2+) (bpy= 2,2'-bipyridine) and a Co4O4 cubane water oxidation catalyst. The two components were assembled either in linear or macrocyclic configurations. In the presence of the sacrificial reagent, the Ru-Co metallocycle exhibits remarkable photocatalytic activity for oxygen evolution, which is one order of magnitude higher than that of a multicomponent system and exceeds that of a linear assembly by a factor of five, offering access to highly active photocatalyst through molecular design.
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