Abstract
AbstractThe complex CuII(Py3P) (1) is an electrocatalyst for water oxidation to dioxygen in H2PO4−/HPO42− buffered aqueous solutions. Controlled potential electrolysis experiments with 1 at pH 8.0 at an applied potential of 1.40 V versus the normal hydrogen electrode resulted in the formation of dioxygen (84 % Faradaic yield) through multiple catalyst turnovers with minimal catalyst deactivation. The results of an electrochemical kinetics study point to a single‐site mechanism for water oxidation catalysis with involvement of phosphate buffer anions either through atom–proton transfer in a rate‐limiting OO bond‐forming step with HPO42− as the acceptor base or by concerted electron–proton transfer with electron transfer to the electrode and proton transfer to the HPO42− base.
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