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- Title
Single-Site Copper(II) Water Oxidation Electrocatalysis: Rate Enhancements with HPO<sub>4</sub><sup>2−</sup> as a Proton Acceptor at pH 8.
- Authors
Coggins, Michael K.; Zhang, Ming ‐ Tian; Chen, Zuofeng; Song, Na; Meyer, Thomas J.
- Abstract
The 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.
- Subjects
ELECTROCATALYSIS; SOLUTION (Chemistry); CHEMICAL reactions; ANALYTICAL chemistry; STANDARD hydrogen electrode
- Publication
Angewandte Chemie, 2014, Vol 126, Issue 45, p12422
- ISSN
0044-8249
- Publication type
Article
- DOI
10.1002/ange.201407131