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Visible light-driven oxygen evolution using a binuclear Ru-bda catalyst
DOI:10.1016/S1872-2067(18)63024-4.png)
摘要
En 中文
Binuclear ruthenium complexes bearing the 2,2'-bipyridine-6,6'-dicarboxylate (bda) ligand have been demonstrated to be highly active catalysts towards water oxidation with Ce-IV as an oxidant. However, the catalytic properties of ruthenium dimers have not yet been explored for visible light-driven water oxidation. Herein, the photocatalytic performance of a dipyridyl propane-bridged ruthenium dimer 2 was investigated in comparison with its monomeric precursor, [Ru(bda)(pic)z] (1), in CH3CN/phosphate buffer mixed solvent in a three -component system including a photosensitizer and a sacrificial electron acceptor. Experimental results showed that the activity of each catalyst was strongly dependent on the content of CH3CN in the phosphate buffer, which not only affected the driving force for water oxidation, but also altered the kinetics of the reaction, probably through different mechanisms associated with the O-O bond formation. As a result, dimer 2 showed significantly higher activity than monomer 1 in the solvent containing a low content of CH3CN, and comparable activities were attained with a high content of CH3CN in the solvent. Under the optimal conditions, complex 2 achieved a turnover number of 638 for photocatalytic O-2 evolution. (C) 2018, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
Keyword:
Water oxidation
Binuclear ruthenium catalyst
Photocatalysis
Solvent effect
Kinetics
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期刊
IF:
17.7
论文数:
4.2K
被引数:
2.1W
机构
引用论文
A molecular ruthenium catalyst with water-oxidation activity comparable to that of photosystem II具有与光系统II相当的水氧化活性的分子钌催化剂
NATURE CHEMISTRY
IF20.2

