催化作用
吸附
解吸
电化学
选择性
电催化剂
密度泛函理论
法拉第效率
材料科学
化学工程
化学
无机化学
物理化学
电极
计算化学
有机化学
工程类
作者
Li Zhu,Yiyang Lin,Kang Liu,Emiliano Cortés,Hongmei Li,Junhua Hu,Akira Yamaguchi,Xiaoliang Liu,Mutsumi Miyauchi,Junwei Fu,Min Liu
出处
期刊:Chinese Journal of Catalysis
[China Science Publishing & Media Ltd.]
日期:2021-09-01
卷期号:42 (9): 1500-1508
被引量:54
标识
DOI:10.1016/s1872-2067(20)63754-8
摘要
Electrochemical CO2 reduction is a promising strategy for utilization of CO2 and intermittent excess electricity. Cu is the only single-metal catalyst that can electrochemically convert CO2 to multi-carbon products. However, Cu has an undesirable selectivity and activity for C2 products, due to its insufficient amount of CO* for C-C coupling. Considering the strong CO2 adsorption and ultra-fast reaction kinetics of CO* formation on Pd, an intimate CuPd(100) interface was designed to lower the intermediate reaction barriers and then improve the efficiency of C2 products. Density functional theory (DFT) calculations showed that the CuPd(100) interface has enhanced CO2 adsorption and decreased CO2* hydrogenation energy barrier, which are beneficial for C-C coupling. The potential-determining step (PDS) barrier of CO2 to C2 products on CuPd(100) interface is 0.61 eV, which is lower than that on Cu(100) (0.72 eV). Motivated by the DFT calculation, the CuPd(100) interface catalyst was prepared by a facile chemical solution method and demonstrated by transmission electron microscope (TEM). The CO2 temperature programmed desorption (CO2-TPD) and gas sensor experiments proved the enhancements of CO2 adsorption and CO2* hydrogenation abilities on CuPd(100) interface catalyst. As a result, the obtained CuPd(100) interface catalyst exhibits a C2 Faradaic efficiency of 50.3 (+/-) 1.2% at -1.4 VRHE in 0.1 M KHCO3, which is 2.1 times higher than 23.6(+/-) 1.5% of Cu catalyst. This work provides a rational design of Cu-based electrocatalyst for multi-carbon products by fine-tuning the intermediate reaction barriers.
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