Selective Tandem CO2-to-C2+Alcohol Conversion at a Single-Crystal Au/Cu Bimetallic Interface

被引:5
|
作者
Zhu, Chenyuan [1 ,2 ]
Zhang, Zhibin [3 ]
Qiao, Ruixi [4 ]
Yang, Chunlei [1 ,2 ]
Zhao, Siwen [1 ,2 ]
Shi, Guoshuai [1 ,2 ]
Gao, Xinyang [1 ,2 ]
Gu, Huoliang [1 ,2 ]
Liu, Kaihui [3 ]
Zhang, Liming [1 ,2 ]
机构
[1] Fudan Univ, iChEM Collaborat Innovat Ctr Chem Energy Mat, Dept Chem, Shanghai 200438, Peoples R China
[2] Fudan Univ, Shanghai Key Lab Mol Catalysis & Innovat Mat, Shanghai 200438, Peoples R China
[3] Peking Univ, Frontiers Sci Ctr Nanooptoelectron, Sch Phys, State Key Lab Mesoscop Phys, Beijing 100871, Peoples R China
[4] Nanjing Univ Aeronaut & Astronaut, Inst Frontier Sci, Nanjing 210016, Peoples R China
关键词
ELECTROCHEMICAL REDUCTION; CARBON-DIOXIDE; CO2; REDUCTION; CU; ELECTROREDUCTION; ELECTRODES; CATALYST; PATHWAYS; INSIGHTS;
D O I
10.1021/acs.jpcc.2c08241
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Copper-based bimetallic heterostructures have recently gained extensive attention because of their promising capability to steer the selectivity of electrochemical CO2 reduction into high-valued multicarbon products. However, a thorough mechanistic under-standing toward the CO2 reduction pathway and the influence of interfacial atomic configuration has not yet been unveiled. Herein, we rationally engaged facet engineering to construct a Au/Cu heterostructure via an epitaxial growth and observed that Au(110)/ Cu(110) exhibited the highest yield rate toward multicarbon alcohols, compared with results for Au(111)/Cu(111) and Au(100)/Cu(100). According to electrochemical analysis, the enhanced activity was attributed to high-conversion capabilities of both CO2-to-CO and *CO-to-C2+ alcohols. Moreover, we confirmed that the buildup of *CO is more crucial than the atomic arrangement of Cu surface for multicarbon production. Our work demonstrates a benchmark tandem CO2 electroreduction system to explicitly link the interfacial atomic configuration to the electrocatalytic performance and sheds light on the facet engineering of bimetallic electrodes in electrolysis.
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收藏
页码:3470 / 3477
页数:8
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