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High CO-tolerant Ru-based catalysts by constructing an oxide blocking layer

journal contribution
posted on 31.05.2022, 13:22 authored by Tao Wang, Lai-Yang Li, Li-Na Chen, Tian Sheng, Luning Chen, Yu-Cheng Wang, Pengyang Zhang, Yu-Hao Hong, Jinyu Ye, Wen-Feng LinWen-Feng Lin, Qinghua Zhang, Peng Zhang, Gang Fu, Na Tian, Shi-Gang Sun, Zhi-You Zhou

CO poisoning of Pt-group metal catalysts is a long-standing problem, particularly for hydrogen oxidation reaction in proton exchange membrane fuel cells. Here, we report a catalyst of Ru oxide-coated Ru supported on TiO2 (Ru@RuO2/TiO2), which can tolerate 1–3% CO, enhanced by about 2 orders of magnitude over the classic PtRu/C catalyst, for hydrogen electrooxidation in a rotating disk electrode test. This catalyst can work stably in 1% CO/H2 for 50 h. About 20% of active sites can survive even in a pure CO environment. The high CO tolerance is not via a traditional bifunctional mechanism, i.e., oxide promoting CO oxidation, but rather via hydrous metal oxide shell blocking CO adsorption. An ab initio molecular dynamics (AIMD) simulation indicates that water confined in grain boundaries of the Ru oxide layer and Ru surface can suppress the diffusion and adsorption of CO. This oxide blocking layer approach opens a promising avenue for the design of high CO-tolerant electrocatalysts for fuel cells.

Funding

National Key Research and Development Program of China (2020YFB1505804)

Natural Science Foundation of China (21875194, 92045302, and 22021001)

History

School

  • Aeronautical, Automotive, Chemical and Materials Engineering

Department

  • Chemical Engineering

Published in

Journal of the American Chemical Society

Volume

144

Issue

21

Pages

9292 - 9301

Publisher

American Chemical Society

Version

AM (Accepted Manuscript)

Rights holder

© American Chemical Society

Publisher statement

This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/jacs.2c00602.

Publication date

2022-05-20

Copyright date

2022

ISSN

0002-7863

eISSN

1520-5126

Language

en

Depositor

Prof Wen Feng Lin. Deposit date: 30 May 2022

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