Chemistry - An Asian Journal
Chemistry - An Asian Journal
5 years ago

Water Oxidation by In Situ Generated [RuII(OH2)(NCNHCO)(pic)2]+

Water Oxidation by In Situ Generated [RuII(OH2)(NCNHCO)(pic)2]+
Fanglin Cai, Cheng Chen, Kui Zhou, Somboon Chaemchuen, Francis Verpoort, Bibimaryam Mousavi, Wei Su
A dinuclear ruthenium complex [RuII(NCNHCO)(pic)2]22+ (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, [RuII(OH2)(NCNHCO)(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. Coordination configuration matters: A Ru dimer, [Ru(NCNHCO)(pic)2]22+ (2), which transforms to two single-site Ru-OH2 species to initiate water oxidation, was prepared and fully characterized. Complex 2 could catalyze water oxidation electrochemically, chemically and photochemically, exhibiting an excellent reactivity and stability.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/asia.201700837

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