Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 34, Pages 18639-18644Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202104020
Keywords
first-row transition metal complexes; reaction mechanisms; redox non-innocent ligand; water oxidation catalysis; water splitting
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Funding
- Ministerio de Ciencia, Innovacion y Universidades
- FEDER [PID2019-111617RB-I00, PID2019-104171RB-I00]
- AGAUR [2017-SGR-1631]
- Ministerio de Ciencia e Inovacion for a Severo Ochoa Excellence Accreditation grant 2020-2023 (MIC/AEI) [CEX2019-000925-S]
- DFG research fellowship [OL-562]
- EU [951843]
- La Caixa Foundation
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This study presents a new family of water oxidation catalyst ligands, and provides experimental and computational evidence supporting an all ligand-based process occurring at pH 11.6.
Water oxidation to dioxygen is one of the key reactions that need to be mastered for the design of practical devices based on water splitting with sunlight. In this context, water oxidation catalysts based on first-row transition metal complexes are highly desirable due to their low cost and their synthetic versatility and tunability through rational ligand design. A new family of dianionic bpy-amidate ligands of general formula H2LNn- (LN is [2,2 '-bipyridine]-6,6 '-dicarboxamide) substituted with phenyl or naphthyl redox non-innocent moieties is described. A detailed electrochemical analysis of [(L4)Cu](2-) (L4=4,4 '-(([2,2 '-bipyridine]-6,6 '-dicarbonyl)bis(azanediyl))dibenzenesulfonate) at pH 11.6 shows the presence of a large electrocatalytic wave for water oxidation catalysis at an eta=830 mV. Combined experimental and computational evidence, support an all ligand-based process with redox events taking place at the aryl-amide groups and at the hydroxido ligands.
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