期刊
ACS CATALYSIS
卷 7, 期 3, 页码 1712-1719出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.6b03253
关键词
water oxidation; water splitting; first row transition metal complexes; DFT; mechanism
资金
- MINECO
- FEDER [CTQ2014-57761-R, CTQ:2016-80058-R, SEV-2013-0319, CTQ:2014-52974-REDC]
- CERCA Programme/Generalitat de Catalunya
- Severo Ochoa predoctoral training fellowship [SVP-2014-0686662]
- La Caixa foundation
The systematic computational study of the mechanism for water oxidation in four different complexes confirms the existence of an alternative mechanism for the O-O bond formation step to those previously reported: the single electron transfer-water nucleophilic attack (SET-WNA). The calculated mechanism relies on two SET steps and features the existence of an intermediate with a (HO center dot center dot center dot OH)(-) moiety in the vicinity of the metal center. It is operative in at least three representative copper based complexes and is the only option that explains the experimentally observed efficiency in two of them. The proposal of this reaction pathway redefines the mechanistic scenario and, importantly, generates a promising avenue for designing more efficient water oxidation catalysts based on first row transition metals.
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