Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 53, Issue 37, Pages 9856-9859Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201402407
Keywords
catalysis; macrocycles; manganese; molecular electrochemistry; water splitting
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Funding
- Indiana University
- American Chemical Society (Petroleum Research Foundation) [50971-ND3]
- U.S. Department of Energy (Office of Basic Energy Sciences) [DE-FG02-08ER15996]
- NIH-RISE [R25 GM06122211]
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The catalytic reactivity of the high-spin Mn-II pyridinophane complexes [(Py2NR2)Mn(H2O)(2)](2+) (R=H, Me, tBu) toward O-2 formation is reported. With small macrocycle N-substituents (R=H, Me), the complexes catalytically disproportionate H2O2 in aqueous solution; with a bulky substituent (R=tBu), this catalytic reaction is shut down, but the complex becomes active for aqueous electrocatalytic H2O oxidation. Control experiments are in support of a homogeneous molecular catalyst and preliminary mechanistic studies suggest that the catalyst is mononuclear. This ligand-controlled switch in catalytic reactivity has implications for the design of new manganese-based water oxidation catalysts.
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