Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 7, Issue 18, Pages 3542-3547Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.6b01235
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Funding
- Chemistry Department at the University of Illinois at Urbana-Champaign
- National Science Foundation [CHE-1309731]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1309731] Funding Source: National Science Foundation
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The development of non-precious-metal (NPM) catalysts to replace the Pt alloys currently used in fuel cells to facilitate the oxygen reduction reaction (ORR) is a vital step in the widespread utilization of fuel cells. Currently, the ORR mechanism for NPM catalysts is not well understood, prohibiting the design and preparation of improved NPM catalysts. We conducted a kinetic isotope effect (KIE) study to identify the rate-determining step (RDS) of this intricate electrocatalytic reaction involving multiple proton-coupled electron transfer (PCET) processes. We observed a KIE of about 2 for the ORR catalyzed by a NPM catalyst, which demonstrates that for these electrocatalysts protons are involved in the RDS during ORR These results contribute to a more complete understanding of the ORR mechanism and suggest that the design of future NPM catalysts must include careful consideration of the role of protons during ORR.
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