New Powerful and Oxidatively Rugged Dinuclear Ru Water Oxidation Catalyst: Control of Mechanistic Pathways by Tailored Ligand Design

New Powerful and Oxidatively Rugged Dinuclear Ru Water Oxidation Catalyst: Control of Mechanistic Pathways by Tailored Ligand Design
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DOI:
10.1021/ja409974b
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发表时间:
2014-01-08
影响因子:
15
通讯作者:
Llobet, Antoni
Llobet, Antoni
中科院分区:
化学1区
文献类型:
--
作者:
Neudeck, Sven;Maji, Somnath;Llobet, Antoni

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制备了一种新的强有力的和抗氧化的吡唑基水氧化催化剂,其式为{[Ru-II(py-SO 3)(2)(H2O)](2)(mu-Mebbp)}(-),1(H2O)(2)(-),并通过光谱和电化学进行了彻底表征。这种新的催化剂是基于特定的配体剪裁设计而构思的,因此其性能得到了系统的改善。它也证明了如何微妙的配体修饰引起的O-O键形成机制的变化,从而揭示了密切的活化能障碍与每个途径。
A new powerful and oxidatively rugged pyrazolate-based water oxidation catalyst of formula {[Ru-II(py-SO3)(2)(H2O)](2)(mu-Mebbp)}(-), 1(H2O)(2)(-), has been prepared and thoroughly characterized spectroscopically and electrochemically. This new catalyst has been conceived based on a specific ligand tailoring design, so that its performance has been systematically improved. It was also demonstrated how subtle ligand modifications cause a change in the O-O bond formation mechanism, thus revealing the close activation energy barriers associated with each pathway.