Asymmetrical C–C Coupling for Electroreduction of CO on Bimetallic Cu–Pd Catalysts
Asymmetrical C–C Coupling for Electroreduction of CO on Bimetallic Cu–Pd Catalysts
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DOI：
10.1021/acscatal.2c00646
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发表时间：
2022-04
期刊：
影响因子：
12.9
通讯作者：
Hao Shen;Yunzhe Wang;Tanmoyendu Chakraborty;Guangye Zhou;Canhui Wang;Xianbiao Fu;Yuxuan Wang;Jinyi Zhang;Chenyang Li;Fei Xu;Liang Cao;Tim Mueller;Chao Wang
中科院分区：
文献类型：
--
作者：
Hao Shen;Yunzhe Wang;Tanmoyendu Chakraborty;Guangye Zhou;Canhui Wang;Xianbiao Fu;Yuxuan Wang;Jinyi Zhang;Chenyang Li;Fei Xu;Liang Cao;Tim Mueller;Chao Wang
Electroreduction of carbon monoxide (CO) possesses great potential for achieving the renewable synthesis of hydrocarbon chemicals from CO2. We report here selective reduction of CO to acetate using Cu–Pd bimetallic electrocatalysts. High activity and selectivity are demonstrated for CO-to-acetate conversion with >200 mA/cm2in geometric current density and >65% in Faradaic efficiency (FE). An asymmetrical C–C coupling mechanism is proposed to explain the composition-dependent catalytic performance and high selectivity toward acetate. This mechanism is supported by the computationally predicted shift of the *CO adsorption from the top-site configuration on Cu (or Cu-rich) surfaces to the bridge sites of Cu–Pd bimetallic surfaces, which is also associated with the reduction of the CO hydrogenation barrier. Further kinetic analysis of the reaction order with respect to CO and Tafel slope supports a reaction pathway with *CO–*CHO recombination following a CO hydrogenation step, which could account for the electroreduction of CO to acetate on the Cu–Pd bimetallic catalysts. Our work highlights how heteroatomic alloy surfaces can be tailored to enable distinct reaction pathways and achieve advanced catalytic performance beyond monometallic catalysts.
