Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 132, Issue 32, Pages 10990-10991Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja104766z
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Funding
- Heinz Endowments
- Charles E. Kaufman Foundation
- R. K. Mellon Foundation
- NSF [CHE-0949238]
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Photolysis of water, a long-studied strategy for storing solar energy, involves two half-reactions: the reduction of protons to dihydrogen and the oxidation of water to dioxygen. Proton reduction is well-understood, with catalysts achieving quantum yields of 34% when driven by visible light. Water oxidation, on the other hand, is much less advanced, typically involving expensive metal centers and rarely working in conjunction with a photochemically powered system. Before further progress can be made in the field of water splitting, significant developments in the catalysis of oxygen evolution are needed. Herein we present an iron-centered tetraamido macrocyclic ligand (Fe-TAML) that efficiently catalyzes the oxidative conversion of water to dioxygen. When the catalyst is combined in unbuffered solution with ceric ammonium nitrate, its turnover frequency exceeds 1.3 s(-1). Real-time UV vis and oxygen monitoring of the active complex give insights into the reaction and decay kinetics.
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