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Tuning the intermediate reaction barriers by a CuPd catalyst to improve the selectivity of CO_(2) electroreduction to C_(2) products

引用

Chinese Journal of Catalysis 2021年第9期42卷 1500-1508页

作者： Li Zhu Yiyang Lin ang Liu Emiliano Cortés Hongmei Li Junhua Hu Akira Yamaguchi Xiaoliang Liu Masahiro Miyauchi Junwei Fu Min Liu Shenzhen Research Institute School of Physics and ElectronicsCentral South UniversityChangsha 410083HunanChina Chair in Hybrid Nanosystems Nanoinstitute MunichFaculty of PhysicsLudwig‐Maximilians‐Universität München80539 MünchenGermany School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450052HenanChina Department of Materials Science and Engineering School of Materials and Chemical TechnologyTokyo Institute of TechnologyTokyo 152‐8552Japan

Electrochemical CO2 reduction is a promising strategy for the utilization of CO2 and intermittent excess *** is the only single metal catalyst that can electrochemically convert CO2 into multicarbon ***,Cu exhibits an unfavorable activity and selectivity for the generation of C2 products because of the insufficient amount of CO*provided for the C‐C *** on the strong CO2 adsorption and ultrafast reaction kinetics of CO*formation on Pd,an intimate CuPd(100)interface was designed to lower the intermediate reaction barriers and improve the efficiency of C2 product *** functional theory(DFT)calculations showed that the CuPd(100)interface enhanced the CO2 adsorption and decreased the CO2*hydrogenation energy barrier,which was beneficial for the C‐C *** potential‐determining step(PDS)barrier of CO2 to C2 products on the CuPd(100)interface was 0.61 eV,which was lower than that on Cu(100)(0.72 eV).Encouraged by the DFT calculation results,the CuPd(100)interface catalyst was prepared by a facile chemical solution method and characterized by transmission electron ***2 temperature‐programmed desorption and gas sensor experiments further confirmed the enhancement of the CO2 adsorption and CO2*hydrogenation ability of the CuPd(100)interface ***,the obtained CuPd(100)interface catalyst exhibited a C2 Faradaic efficiency of 50.3%±1.2%at‒1.4 VRHE in 0.1 M KHCO3,which was 2.1 times higher than that of the Cu catalyst(23.6%±1.5%).This study provides the basis for the rational design of Cu‐based electrocatalysts for the generation of multicarbon products by fine‐tuning the intermediate reaction barriers.

关键词： Carbon dioxide reduction C2 products Electrocatalyst Copper‐palladium interface intermediate reaction barriers

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