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Water Oxidation by In Situ Generated [Ru II (OH 2 )(NC NHC O)(pic) 2 ] +
Author(s) -
Su Wei,
Zhou Kui,
Cai Fanglin,
Chen Cheng,
Mousavi Bibimaryam,
Chaemchuen Somboon,
Verpoort Francis
Publication year - 2017
Publication title -
chemistry – an asian journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.18
H-Index - 106
eISSN - 1861-471X
pISSN - 1861-4728
DOI - 10.1002/asia.201700837
Subject(s) - ruthenium , catalysis , chemistry , ligand (biochemistry) , oxidation state , proton , electron transfer , photochemistry , redox , inorganic chemistry , physics , receptor , quantum mechanics , biochemistry
A dinuclear ruthenium complex [Ru II (NC NHC O)(pic) 2 ] 2 2+ ( 2 ) was firstly prepared and characterized spectroscopically and electrochemically. Instead of the conventional ligand exchange, complex 2 dissociates in situ to afford two single‐site Ru aqua complexes, [Ru II (OH 2 )(NC NHC O)(pic) 2 ] + , which mediates water oxidation through proton‐coupled electron transfer events. In electrokinetic studies, complex 2 demonstrated a TOF of 150.3 s −1 comparable to those state‐of‐the‐art catalysts at neutral conditions. TONs of 2173 and 217 were attained in chemical and photochemical water oxidation when 2 was used as a catalyst, exhibiting good stability. Notably, a TOF of 1.3 s −1 was achieved at CAN‐driven water oxidation, which outperformed most of the reported single‐site Ru complexes, indicating that complex 2 is one of most active water oxidation catalysts (WOCs) to date. The unique coordination configuration and outstanding catalytic performance of complex 2 might shed light on the design of novel molecular WOCs.