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Tse EC, Varnell JA, Hoang TT, et al. Elucidating Proton Involvement in the Rate-Determining Step for Pt/Pd-Based and Non-Precious-Metal Oxygen Reduction Reaction Catalysts Using the Kinetic Isotope Effect. J Phys Chem Lett. 2016;7(18):3542-7doi: 10.1021/acs.jpclett.6b01235.
Tse, E. C., Varnell, J. A., Hoang, T. T., & Gewirth, A. A. (2016). Elucidating Proton Involvement in the Rate-Determining Step for Pt/Pd-Based and Non-Precious-Metal Oxygen Reduction Reaction Catalysts Using the Kinetic Isotope Effect. The journal of physical chemistry letters, 7(18), 3542-7. https://doi.org/10.1021/acs.jpclett.6b01235
Tse, Edmund C M, et al. "Elucidating Proton Involvement in the Rate-Determining Step for Pt/Pd-Based and Non-Precious-Metal Oxygen Reduction Reaction Catalysts Using the Kinetic Isotope Effect." The journal of physical chemistry letters vol. 7,18 (2016): 3542-7. doi: https://doi.org/10.1021/acs.jpclett.6b01235
Tse EC, Varnell JA, Hoang TT, Gewirth AA. Elucidating Proton Involvement in the Rate-Determining Step for Pt/Pd-Based and Non-Precious-Metal Oxygen Reduction Reaction Catalysts Using the Kinetic Isotope Effect. J Phys Chem Lett. 2016 Sep 15;7(18):3542-7. doi: 10.1021/acs.jpclett.6b01235. Epub 2016 Aug 26. PMID: 27550191.
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J Phys Chem Lett. 2016 Sep 15;7(18):3542-7. doi: 10.1021/acs.jpclett.6b01235. Epub 2016 Aug 26.

Elucidating Proton Involvement in the Rate-Determining Step for Pt/Pd-Based and Non-Precious-Metal Oxygen Reduction Reaction Catalysts Using the Kinetic Isotope Effect.

The journal of physical chemistry letters

Edmund C M Tse, Jason A Varnell, Thao T H Hoang, Andrew A Gewirth

Affiliations

  1. Department of Chemistry, University of Illinois at Urbana-Champaign , Urbana, Illinois 61801, United States.
  2. International Institute for Carbon Neutral Energy Research (WPI-I2CNER), Kyushu University , Fukuoka 812-8581, Japan.

PMID: 27550191 DOI: 10.1021/acs.jpclett.6b01235

Abstract

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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