Atomically Dispersed CrOX on Pd Metallene for CO-Resistant Methanol Oxidation

Yu Qiu; Jinchang Fan; Jiandong Wu; Wenting Lu; Shengwei Wang; Dewen Wang; Xin Ge; Xiao Zhao; Wei Zhang; Weitao Zheng; Xiaoqiang Cui

doi:10.1021/acs.nanolett.3c03141

Atomically Dispersed CrO_X on Pd Metallene for CO-Resistant Methanol Oxidation

Nano Lett. 2023 Oct 25;23(20):9555-9562. doi: 10.1021/acs.nanolett.3c03141. Epub 2023 Oct 3.

Authors

Yu Qiu¹, Jinchang Fan¹, Jiandong Wu^{1

2}, Wenting Lu¹, Shengwei Wang³, Dewen Wang¹, Xin Ge¹, Xiao Zhao¹, Wei Zhang¹, Weitao Zheng¹, Xiaoqiang Cui¹

Affiliations

¹ State Key Laboratory of Automotive Simulation and Control, School of Materials Science and Engineering, Key Laboratory of Automobile Materials of MOE, Jilin University, 2699 Qianjin Street, Changchun 130012, People's Republic of China.
² Key Laboratory of Pathobiology of MOE, Nanomedicine and Translational Research Center, The Third Bethune Hospital of Jilin University, 126 Sendai Street, Changchun 130033, People's Republic of China.
³ State Key Laboratory of Automotive Simulation and Control, School of Materials Science and Engineering, Key Laboratory of Automobile Materials of MOE, Jilin University, 5988 Renmin Street, Changchun 130025, People's Republic of China.

PMID: 37787483
DOI: 10.1021/acs.nanolett.3c03141

Abstract

The effective design and construction of high-performance methanol oxidation reaction (MOR) electrocatalysts are significant for the development of direct methanol fuel cells. But the active sites of the MOR electrocatalysts are susceptible to being poisoned by CO, resulting in poor durability. Herein, we report an atomically dispersed CrO_X species anchored on Pd metallene through bridging O atoms. This catalyst shows an outstanding MOR performance with 7 times higher mass activity and 100 mV lower CO electrooxidation potential than commercial Pd/C. The results of operando electrochemical Fourier transform infrared spectroscopy demonstrate the rapid removal of CO* on CrO_X-Pd metallene. Theoretical calculations reveal that atomically dispersed CrO_X can lower the adsorption energy of CO* on Pd sites and enhance that of OH* through the formation of a hydrogen bond, decreasing the formation energy of COOH*. This work provides a new strategy for improving MOR performance via atomically engineering oxide/metal interfaces.

Keywords: CO-resistant; CrOX; electrocatalyst; metallene; methanol oxidation.