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Atomically Dispersed CrO X on Pd Metallene for CO-Resistant Methanol Oxidation

作者:Yu Qiu, Jinchang Fan, Jiandong Wu, Wenting Lu, Shengwei Wang, Dewen Wang, Xin Ge, Xiao Zhao, Wei Zhang, Weitao Zheng, Xiaoqiang Cui · 发表于:Nano Letters · 年份:2023 · DOI:10.1021/acs.nanolett.3c03141 · 被引用次数:42 · 研究领域:Electrocatalysts for Energy Conversion、Catalytic Processes in Materials Science、Advanced battery technologies research

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.