Ligand Modification Transforms a Catalase Mimic into a Water Oxidation Catalyst†
Dr. Wei-Tsung Lee
Department of Chemistry, Indiana University, 800 East Kirkwood Ave., Bloomington, IN 47405 (USA)
Search for more papers by this authorSalvador B. Muñoz III
Department of Chemistry, Indiana University, 800 East Kirkwood Ave., Bloomington, IN 47405 (USA)
Search for more papers by this authorDr. Diane A. Dickie
Department of Chemistry and Chemical Biology, The University of New Mexico, Albuquerque, NM 87131 (USA)
Search for more papers by this authorCorresponding Author
Prof. Jeremy M. Smith
Department of Chemistry, Indiana University, 800 East Kirkwood Ave., Bloomington, IN 47405 (USA)
Department of Chemistry, Indiana University, 800 East Kirkwood Ave., Bloomington, IN 47405 (USA)Search for more papers by this authorDr. Wei-Tsung Lee
Department of Chemistry, Indiana University, 800 East Kirkwood Ave., Bloomington, IN 47405 (USA)
Search for more papers by this authorSalvador B. Muñoz III
Department of Chemistry, Indiana University, 800 East Kirkwood Ave., Bloomington, IN 47405 (USA)
Search for more papers by this authorDr. Diane A. Dickie
Department of Chemistry and Chemical Biology, The University of New Mexico, Albuquerque, NM 87131 (USA)
Search for more papers by this authorCorresponding Author
Prof. Jeremy M. Smith
Department of Chemistry, Indiana University, 800 East Kirkwood Ave., Bloomington, IN 47405 (USA)
Department of Chemistry, Indiana University, 800 East Kirkwood Ave., Bloomington, IN 47405 (USA)Search for more papers by this authorFunding from Indiana University, the American Chemical Society (Petroleum Research Foundation, 50971-ND3), and the U.S. Department of Energy (Office of Basic Energy Sciences; DE-FG02-08ER15996) is gratefully acknowledged. J.M.S. is a Dreyfus Teacher-Scholar. S.B.M. acknowledges support from NIH-RISE (R25 GM06122211). We thank Song Xu, Dennis Chen, and Sara Skrabalak for experimental assistance.
Graphical Abstract
Ligand-controlled switch: Simple modification of the substituent on a pyridinophane macrocycle ligand converts the corresponding MnII complex from a hydrogen peroxide disproportionation catalyst into a water oxidation catalyst. Preliminary results indicate that the catalyst is mononuclear.
Abstract
The catalytic reactivity of the high-spin MnII pyridinophane complexes [(Py2NR2)Mn(H2O)2]2+ (R=H, Me, tBu) toward O2 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.
Supporting Information
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