Interfacial Synergy between the Cu Atomic Layer and CeO2 Promotes CO Electrocoupling to Acetate

被引:39
|
作者
Yang, Tang [1 ]
Lin, Li [1 ]
Lv, Ximeng [2 ]
Yang, Hongcen [3 ]
Feng, Huishu [1 ]
Huang, Zhongliang [1 ]
Li, Jiwei [1 ]
Pao, Chih-Wen [4 ]
Hu, Zhiwei [5 ]
Zhan, Changhong [1 ]
Xu, Yong [6 ]
Zheng, Lan-Sun [1 ]
Jiao, Feng [7 ]
Huang, Xiaoqing [1 ]
机构
[1] Xiamen Univ, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China
[2] Fudan Univ, Fac Chem & Mat Sci, Dept Chem, Lab Adv Mat, Shanghai 200438, Peoples R China
[3] Lanzhou Univ, Sch Mat & Energy, Natl & Local Joint Engn Lab Opt Convers Mat & Tech, Lanzhou 730000, Peoples R China
[4] Natl Synchrotron Radiat Res Ctr, Hsinchu 30076, Taiwan
[5] Max Planck Inst Chem Phys Solids, D-01187 Dresden, Germany
[6] Guangdong Univ Technol, Collaborat Innovat Ctr Adv Energy Mat, Sch Mat & Energy, Guangzhou Key Lab Low Dimens Mat & Energy Storage, Guangzhou 510006, Peoples R China
[7] Univ Delaware, Ctr Catalyt Sci & Technol, Dept Chem & Biomol Engn, Newark, DE 19716 USA
基金
中国国家自然科学基金; 中国博士后科学基金; 国家重点研发计划;
关键词
synergy; Cu atomic layer; CO reduction reaction; acetate selectivity; stability; CARBON-MONOXIDE; ELECTROCHEMICAL REDUCTION; ELECTROREDUCTION; PRODUCTS; COPPER; DIOXIDE; FUEL;
D O I
10.1021/acsnano.3c00817
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Cu is considered to be an effective electrocatalyst in CO/CO2 reduction reactions (CORR/CO2RR) because of its C-C coupling into C2+ products, but it still remains a formidable challenge to rationally design Cu-based catalysts for highly selective CO/CO2 reduction to C2+ liquid products such as acetate. We here demonstrate that spraying atomically layered Cu atoms onto CeO2 nanorods (Cu-CeO2) can lead to a catalyst with an enhanced acetate selectivity in CORR. Owing to the existence of oxygen vacancies (Ov) in CeO2, the layer of Cu atoms at interface coordinates with Ce atoms in the form of Cu- Ce (Ov), as a result of strong interfacial synergy. The Cu-Ce (Ov) significantly promotes the adsorption and dissociation of H2O, which further couples with CO to selectively produce acetate as the dominant liquid product. In the current density range of 50-150 mA cm-2, the Faradaic efficiencies (FEs) of acetate are over 50% with a maximum value of 62.4%. In particular, the turnover frequency of Cu-CeO2 reaches 1477 h-1, surpassing that of Cu nanoparticle-decorated CeO2 nanorods, bare CeO2 nanorods, as well as other existing Cu-based catalysts. This work advances the rational design of high-performance catalysts for CORR to highly value-added products, which may attract great interests in diverse fields including materials science, chemistry, and catalysis.
引用
收藏
页码:8521 / 8529
页数:9
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