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

作     者：Li Zhu Yiyang Lin ang Liu Emiliano Cortés Hongmei Li Junhua Hu Akira Yamaguchi Xiaoliang Liu Masahiro Miyauchi Junwei Fu Min Liu 朱莉;林翌阳;刘康;Emiliano Cortés;李红梅;胡俊华;Akira Yamaguchi;刘小良;Masahiro Miyauchi;傅俊伟;刘敏

作者机构：Shenzhen Research InstituteSchool of Physics and ElectronicsCentral South UniversityChangsha 410083HunanChina Chair in Hybrid NanosystemsNanoinstitute MunichFaculty of PhysicsLudwig‐Maximilians‐Universität München80539 MünchenGermany School of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450052HenanChina Department of Materials Science and EngineeringSchool of Materials and Chemical TechnologyTokyo Institute of TechnologyTokyo 152‐8552Japan 

出 版 物：《Chinese Journal of Catalysis》 (催化学报（英文）)

年 卷 期：2021年第42卷第9期

页      面：1500-1508页

核心收录：

学科分类：081702[工学-化学工艺] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 080502[工学-材料学] 0805[工学-材料科学与工程（可授工学、理学学位）] 

基　　金：国家自然科学基金(21872174,22002189,51673217,U1932148) 国家科技部重点研发国际间合作项目(2017YFE0127800,2018YFE 0203402) 湖南省科技计划项目(2017XK2026) 湖南省自然科学基金(2020JJ2041,2020JJ5691),湖南省科技计划项目(2017TP1001) 深圳科技创新项目(JCYJ20180307151313532) 

主　　题：Carbon dioxide reduction C2 products Electrocatalyst Copper‐palladium interface Intermediate reaction barriers 

摘      要：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.