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Communication

Electrocatalytic O₂ Reduction by Covalently Immobilized Mononuclear Copper(I) Complexes: Evidence for a Binuclear Cu₂O₂ Intermediate

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Charles C. L. McCrory, Anando Devadoss, Xavier Ottenwaelder, Randall D. Lowe, T. Daniel P. Stack*, and Christopher E. D. Chidsey*

Department of Chemistry, Stanford University, Stanford, California 94305, United States

J. Am. Chem. Soc., 2011, 133 (11), pp 3696–3699

DOI: 10.1021/ja106338h

Publication Date (Web): March 2, 2011

stack@stanford.edu; chidsey@stanford.edu

† Author Present Address

Department of Chemistry, California Institute of Technology, Pasadena, CA 91125

‡ Author Present Address

Hitachi Chemical Research Center, Inc., Irvine, CA 92617

§ Author Present Address

Department of Chemistry and Biochemistry, Concordia University, Montreal, Quebec, Canada H4B 1R6

Section:

Electrochemistry

Abstract

A Cu^I complex of 3-ethynyl-phenanthroline covalently immobilized onto an azide-modified glassy carbon surface is an active electrocatalyst for the four-electron (4-e) reduction of O₂ to H₂O. The rate of O₂ reduction is second-order in Cu coverage at moderate overpotential, suggesting that two Cu^I species are necessary for efficient 4-e reduction of O₂. Mechanisms for O₂ reduction are proposed that are consistent with the observations for this covalently immobilized system and previously reported results for a similar physisorbed Cu^I system.

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History

Published In Issue March 23, 2011
Article ASAPMarch 02, 2011
Received: July 16, 2010

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