Sharp Cu@Sn nanocones on Cu foam for highly selective and efficient electrochemical reduction of CO2 to formate

被引:76
作者
Chen, Chengzhen [1 ]
Pang, Yuanjie [2 ]
Zhang, Fanghua [1 ]
Zhong, Juhua [3 ]
Zhang, Bo [4 ]
Cheng, Zhenmin [1 ]
机构
[1] East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China
[2] Huazhong Univ Sci & Technol, Sch Opt & Elect Informat, Wuhan 430074, Hubei, Peoples R China
[3] East China Univ Sci & Technol, Dept Phys, Shanghai 200237, Peoples R China
[4] Fudan Univ, Dept Macromol Sci, State Key Lab Mol Engn Polymers, Shanghai 200438, Peoples R China
关键词
CARBON-DIOXIDE REDUCTION; FORMIC-ACID; AQUEOUS CO2; HIGH-DENSITY; ELECTROREDUCTION; CATALYSTS; ELECTRODES; NANOPARTICLES; ELECTROCATALYST; CONVERSION;
D O I
10.1039/c8ta06826g
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
Electrochemical reduction of aqueous CO2 into formate is subject to poor selectivity and low current density with conventional Sn-based catalysts owing to the inert nature of CO2 molecules and the low number of active sites. Recently, it has been demonstrated that alkali metal cations could greatly enhance selectivity for CO2 reduction by stabilizing the key intermediates, which leads to an effective solution to this problem by concentrating local metal cations through tailoring the catalyst structure. Herein, we synthesized spiky Cu@Sn nanocones over a macroporous Cu foam, which has a curvature radius of 10nm, via facile electrochemical coating of a thin layer of Sn over the Cu nanoconic surface. A faradaic efficiency of 90.4% toward formate production was achieved, with a current density of 57.7 mA cm(-2) at -1.1 V vs. a reversible hydrogen electrode, which far exceeds results achieved to date with state-of-the-art Sn catalysts. The performance should be attributed to the combined effects of a sharp conical feature that facilitates the enrichment of surface-adsorbed metal cations and the promotion of the mass transfer and active sites growth favored by the three-dimensional porous network.
引用
收藏
页码:19621 / 19630
页数:10
相关论文
共 48 条
[1]   Nanostructured transition metal dichalcogenide electrocatalysts for CO2 reduction in ionic liquid [J].
Asadi, Mohammad ;
Kim, Kibum ;
Liu, Cong ;
Addepalli, Aditya Venkata ;
Abbasi, Pedram ;
Yasaei, Poya ;
Phillips, Patrick ;
Behranginia, Amirhossein ;
Cerrato, Jose M. ;
Haasch, Richard ;
Zapol, Peter ;
Kumar, Bijandra ;
Klie, Robert F. ;
Abiade, Jeremiah ;
Curtiss, Larry A. ;
Salehi-Khojin, Amin .
SCIENCE, 2016, 353 (6298) :467-470
[2]   Exclusive Formation of Formic Acid from CO2 Electroreduction by a Tunable Pd-Sn Alloy [J].
Bai, Xiaofang ;
Chen, Wei ;
Zhao, Chengcheng ;
Li, Shenggang ;
Song, Yanfang ;
Ge, Ruipeng ;
Wei, Wei ;
Sun, Yuhan .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2017, 56 (40) :12219-12223
[3]   Selective electrochemical CO2 reduction over highly porous gold films [J].
Chen, Chengzhen ;
Zhang, Bo ;
Zhong, Juhua ;
Cheng, Zhenmin .
JOURNAL OF MATERIALS CHEMISTRY A, 2017, 5 (41) :21955-21964
[4]   Electric Field Effects in Electrochemical CO2 Reduction [J].
Chen, Leanne D. ;
Urushihara, Makoto ;
Chan, Karen ;
Norskov, Jens K. .
ACS CATALYSIS, 2016, 6 (10) :7133-7139
[5]   Aqueous CO2 Reduction at Very Low Overpotential on Oxide-Derived Au Nanoparticles [J].
Chen, Yihong ;
Li, Christina W. ;
Kanan, Matthew W. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (49) :19969-19972
[6]   Tin Oxide Dependence of the CO2 Reduction Efficiency on Tin Electrodes and Enhanced Activity for Tin/Tin Oxide Thin-Film Catalysts [J].
Chen, Yihong ;
Kanan, Matthew W. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (04) :1986-1989
[7]   Surface engineered tin foil for electrocatalytic reduction of carbon dioxide to formate [J].
Daiyan, Rahman ;
Lu, Xunyu ;
Ng, Yun Hau ;
Amal, Rose .
CATALYSIS SCIENCE & TECHNOLOGY, 2017, 7 (12) :2542-2550
[8]   Partially oxidized atomic cobalt layers for carbon dioxide electroreduction to liquid fuel [J].
Gao, Shan ;
Lin, Yue ;
Jiao, Xingchen ;
Sun, Yongfu ;
Luo, Qiquan ;
Zhang, Wenhua ;
Li, Dianqi ;
Yang, Jinlong ;
Xie, Yi .
NATURE, 2016, 529 (7584) :68-+
[9]   Mesostructure-Induced Selectivity in CO2 Reduction Catalysis [J].
Hall, Anthony Shoji ;
Yoon, Youngmin ;
Wuttig, Anna ;
Surendranath, Yogesh .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2015, 137 (47) :14834-14837
[10]   Effect of Chloride Anions on the Synthesis and Enhanced Catalytic Activity of Silver Nanocoral Electrodes for CO2 Electroreduction [J].
Hsieh, Yu-Chi ;
Senanayake, Sanjaya D. ;
Zhang, Yu ;
Xu, Wenqian ;
Polyansky, Dmitry E. .
ACS CATALYSIS, 2015, 5 (09) :5349-5356