Engineering Cu(I)/Cu(0) interfaces for efficient ethanol production from CO2 electroreduction

被引:68
作者
Cai, Rongming [1 ,2 ]
Sun, Mingzi [3 ]
Yang, Fei [4 ]
Gu, Danny
Ju, Min [1 ]
Chen, Yanpeng [1 ]
Gu, M. Danny [4 ]
Huang, Bolong [3 ,5 ]
Yang, Shihe [1 ,2 ]
机构
[1] Peking Univ, Sch Chem Biol & Biotechnol, Shenzhen Grad Sch, Guangdong Prov Key Lab Nanomicro Mat Res, Shenzhen 518055, Peoples R China
[2] Inst Biomed Engn, Shenzhen Bay Lab, Shenzhen 518107, Peoples R China
[3] Hong Kong Polytech Univ, Dept Appl Biol & Chem Technol, Hung Hom, Kowloon, Hong Kong, Peoples R China
[4] Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China
[5] Hong Kong Polytech Univ, Res Ctr Carbon Strateg Catalysis RC CSC, Hung Hom, Kowloon, Hong Kong, Peoples R China
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
Cu(I)/Cu(0) nanodisk; Cu(0) Interface region; Cu(I)/Cu(0) interface model; Cu(0) sites; GENERALIZED GRADIENT APPROXIMATION; ELECTROCHEMICAL REDUCTION; CARBON-DIOXIDE; SELECTIVITY; CATALYSTS;
D O I
10.1016/j.chempr.2023.08.027
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
By leveraging a Cu(OH)F precursor, we construct a disk -like Cu(I)/ Cu(0) interface model (P-Cux/Cu2OF) composed of F -stabilized Cu(I) shell and Cu(0) core by one-step pulsed potential conversion. The interfacial region is shown to facilitate ethanol formation, guaranteeing a high FE(C2+) of up to 80.2%. Tuning the Cu(I)/Cu(0) ratio enhances the ethanol yield by 18.5 -fold over pure P -Cu, with the corresponding partial current density (jethanol) reaching up to 128 mA/cm2. This is enabled by a 3.6 -fold boost in selectivity for the ethanol product (35.4%) and an overall 7.8 -fold boost in activity (jC2+up to 288 mA/cm2). The interactions between P -Cu and Cu2OF upshift the d -band center of Cu sites on the interface region, which is critical to asymmetrical C -C coupling to form OCCOH*, concurrent with a lowered energy barrier for ethanol formation. On the other hand, the ethylene -forming symmetrical C -C coupling occurs primarily on P -Cu away from the Cu(I)/Cu(0) interface.
引用
收藏
页码:211 / 233
页数:24
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