Modulation of *CHXO Adsorption to Facilitate Electrocatalytic Reduction of CO2 to CH4 over Cu-Based Catalysts

被引:119
作者
Zhao, Jing [1 ,2 ]
Zhang, Peng [1 ,2 ,3 ]
Yuan, Tenghui [1 ,2 ]
Cheng, Dongfang [1 ,2 ]
Zhen, Shiyu [1 ,2 ]
Gao, Hui [1 ,2 ]
Wang, Tuo [1 ,2 ,3 ,4 ]
Zhao, Zhi-Jian [1 ,2 ,3 ]
Gong, Jinlong [1 ,2 ,3 ,5 ]
机构
[1] Tianjin Univ, Minist Educ, Sch Chem Engn & Technol, Key Lab Green Chem Technol, Tianjin 300072, Peoples R China
[2] Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300072, Peoples R China
[3] Tianjin Univ, Natl Ind Educ Platform Energy Storage, Tianjin 300350, Peoples R China
[4] Joint Sch Natl Univ Singapore & Tianjin Univ, Int Campus Tianjin Univ, Binhai New City 350207, Peoples R China
[5] Haihe Lab Sustainable Chem Transformat, Tianjin 300192, Peoples R China
基金
国家重点研发计划; 中国国家自然科学基金;
关键词
CARBON-DIOXIDE; SURFACE; ELECTROREDUCTION; OXOPHILICITY; SPECTROSCOPY; IONS;
D O I
10.1021/jacs.2c12006
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Copper (Cu) can efficiently catalyze the electrochemical CO2 reduction reaction (CO2RR) to produce value-added fuels and chemicals, among which methane (CH4) has drawn attention due to its high mass energy density. However, the linear scaling relationship between the adsorption energies of *CO and *CHxO on Cu restricts the selectivity toward CH4. Alloying a secondary metal in Cu provides a new freedom to break the linear scaling relationship, thus regulating the product distribution. This paper describes a controllable electrodeposition approach to alloying Cu with oxophilic metal (M) to steer the reaction pathway toward CH4. The optimized La5Cu95 electrocatalyst exhibits a CH4 Faradaic efficiency of 64.5%, with the partial current density of 193.5 mA cm-2. The introduction of oxophilic La could lower the energy barrier for *CO hydrogenation to *CHxO by strengthening the M-O bond, which would also promote the breakage of the C-O bond in *CH3O for the formation of CH4. This work provides a new avenue for the design of Cu-based electrocatalysts to achieve high selectivity in CO2RR through the modulation of the adsorption behaviors of key intermediates.
引用
收藏
页码:6622 / 6627
页数:6
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