Single-Molecule Nanocatalysis Shows In Situ Deactivation of Pt/C Electrocatalysts during the Hydrogen-Oxidation Reaction

Yuwei Zhang; Tao Chen; Shaun Alia; Bryan S Pivovar; Weilin Xu

doi:10.1002/anie.201511071

Single-Molecule Nanocatalysis Shows In Situ Deactivation of Pt/C Electrocatalysts during the Hydrogen-Oxidation Reaction

Angew Chem Int Ed Engl. 2016 Feb 24;55(9):3086-90. doi: 10.1002/anie.201511071. Epub 2016 Jan 28.

Authors

Yuwei Zhang^{1

2}, Tao Chen^{1

2

3}, Shaun Alia⁴, Bryan S Pivovar⁴, Weilin Xu^{5

6}

Affiliations

¹ State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Science, 5625 Renmin Street, Changchun, 130022, P.R. China.
² Jilin Province Key Laboratory of Low Carbon Chemical Power, Changchun Institute of Applied Chemistry, Chinese Academy of Science, 5625 Renmin Street, Changchun, 130022, P.R. China.
³ Graduate University of Chinese Academy of Science, Beijing, 100049, China.
⁴ National Renewable Energy Laboratory, Golden, CO, 80401, USA.
⁵ State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Science, 5625 Renmin Street, Changchun, 130022, P.R. China. weilinxu@ciac.ac.cn.
⁶ Jilin Province Key Laboratory of Low Carbon Chemical Power, Changchun Institute of Applied Chemistry, Chinese Academy of Science, 5625 Renmin Street, Changchun, 130022, P.R. China. weilinxu@ciac.ac.cn.

PMID: 26821777
DOI: 10.1002/anie.201511071

Abstract

By coupling a Pt-catalyzed fluorogenic reaction with the Pt-electrocatalyzed hydrogen-oxidation reaction (HOR), we combine single-molecule fluorescence microscopy with traditional electrochemical methods to study the real-time deactivation kinetics of a Pt/C electrocatalyst at single-particle level during electrocatalytic hydrogen-oxidation reaction. The decay of the catalytic performance of Pt/C could be mainly attributed to the electrocatalysis-induced etching or dissolution of Pt nanoparticles. Spontaneous regeneration of activity and incubation period of the Pt electrocatalyst were also observed at single-particle level. All these new insights are practically useful for the understanding and rational design of highly efficient electrocatalysts for application in fuel cells.

Keywords: deactivation; electrocatalysis; electrochemistry; platinum; single-molecule fluorescence.

Publication types

Research Support, Non-U.S. Gov't