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A Self-Improved Water-Oxidation Catalyst: Is One Site Really Enough?
Citation key Lopez2014
Author Lopez, Isidoro and Ertem, Mehmed Z. and Maji, Somnath and Benet-Buchholz, Jordi and Keidel, Anke and Kuhlmann, Uwe and Hildebrandt, Peter and Cramer, Christopher J. and Batista, Victor S. and Llobet, Antoni
Pages 205–209
Year 2014
DOI 10.1002/anie.201307509
Journal Angewandte Chemie-international Edition
Volume 53
Number 1
Abstract 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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