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The Bifurcation Point of the Oxygen Reduction Reaction on Au-Pd Nanoalloys

Journal article
Authors Jakub Staszak-Jirkovský
Elisabet Ahlberg
Itai Panas
David J Schiffrin
Published in Faraday discussions
Volume 188
Pages 257-278
ISSN 1364-5498
Publication year 2016
Published at Department of Chemistry and Molecular Biology
Pages 257-278
Language en
Links dx.doi.org/10.1039/c5fd00233h
Keywords Hydrogen peroxide synthesis, oxygen reduction, nanoalloys, Au-Pd catalysts, electrocatalysis
Subject categories Electrochemistry, Kinetics, Quantum chemistry

Abstract

The oxygen reduction reaction is of major importance in energy conversion and storage. Controlling electrocatalytic activity and its selectivity remains a challenge of modern electrochemistry. Here, first principle calculations and analysis of experimental data unravel the mechanism of this reaction on Au-Pd nanoalloys in acid media. A mechanistic model is proposed from comparison of electrocatalysis of oxygen and hydrogen peroxide reduction on different Au-Pd ensembles. A H2O production channel on contiguous Pd sites proceeding through intermediates different from H2O2 and OOHσ adsorbate is identified as the bifurcation point for the two reaction pathway alternatives to yield either H2O or H2O2. H2O2 is a leaving group, albeit reduction of H2O2 to H2O can occur by electrocatalytic HO-OH dissociation that is affected by the presence of adsorbed OOHσ. Similarities and differences between electrochemical and direct synthesis from H2 + O2 reaction on Au-Pd nanoalloys are discussed.

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