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Water oxidation catalyzed by a charge-neutral mononuclear ruthenium(III) complex

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Indexed by:期刊论文

Date of Publication:2017-01-01

Journal:DALTON TRANSACTIONS

Included Journals:SCIE、EI、PubMed

Volume:46

Issue:4

Page Number:1304-1310

ISSN No.:1477-9226

Abstract:A new charge-neutral Ru(III) complex RuL(pic)(3) (1) (H3L = 3,6-di-tert-butyl-9H-carbazole-1,8-dicarboxylic acid, pic = 4-picoline) was synthesized and fully characterized. This complex promoted chemical and photochemical water oxidation efficiently with turnover frequencies of 0.28 s(-1) and 5 min(-1), respectively. In particular, for photochemical water oxidation, complex 1 showed excellent stability and good activity. The X-ray crystal structure, electrochemical results, and the detection of the Ru-IV-OH intermediate by high-resolution mass spectrometry revealed that complex 1 exchanged its 4-picoline ligand with water at the Ru-III state to form the authentic water oxidation catalyst. The kinetics studies suggested a reaction mechanism involving nucleophilic attack by a water molecule.

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