Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 53, Issue 1, Pages 205-209Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201307509
Keywords
density functional calculations; reaction mechanisms; resonance Raman spectroscopy; ruthenium electrochemistry; water-oxidation catalysis
Categories
Funding
- MINECO [CTQ2010-21497, PRI-PIBIN-2011-1278]
- FPU
- Torres Quevedo
- Cluster of Excellence (UniCat)
- US Department of Energy (DOE) [DE-SC0001423]
- Computational Materials and Chemical Sciences (CMCSN) project at Brookhaven National Laboratory with the US DOE [DE-AC02-98CH10886]
- Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences
- US National Science Foundation [CHE-0952054]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [0952054] Funding Source: National Science Foundation
- U.S. Department of Energy (DOE) [DE-SC0001423] Funding Source: U.S. Department of Energy (DOE)
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The homogeneous catalysis of water oxidation by transition-metal complexes has experienced spectacular development over the last five years. Practical energy-conversion schemes, however, require robust catalysts with large turnover frequencies. Herein we introduce a new oxidatively rugged and powerful dinuclear water-oxidation catalyst that is generated by self-assembly from a mononuclear catalyst during the catalytic process. Our kinetic and DFT computational analysis shows that two interconnected catalytic cycles coexist while the mononuclear system is slowly and irreversibly converted into the more stable dinuclear system: an extremely robust water-oxidation catalyst that does not decompose over extended periods of time.
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