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Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599,United States
J. Am. Chem. Soc., Article ASAP
DOI: 10.1021/ja412822u
Publication Date (Web): March 26, 2014
Copyright © 2014 American Chemical Society
Abstract
The six-coordinate FeIII-aqua complex [FeIII(dpaq)(H2O)]2+ (1, dpaq is 2-[bis(pyridine-2-ylmethyl)]amino-N-quinolin-8-yl-acetamido) is an electrocatalyst for water oxidation in propylene carbonate–water mixtures. An electrochemical kinetics study has revealed that water oxidation occurs by oxidation to FeV(O)2+ followed by a reaction first order in catalyst and added water, respectively, with ko = 0.035(4) M–1 s–1 by the single-site mechanism found previously for Ru and Ir water oxidation catalysts. Sustained water oxidation catalysis occurs at a high surface area electrode to give O2 through at least 29 turnovers over an 15 h electrolysis period with a 45% Faradaic yield and no observable decomposition of the catalyst.
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