Interfaced Ag/Cu nanostructures derived from metal thiolate nanoplates: A highly selective catalyst for electrochemical reduction of CO2 to ethanol

被引:20
作者
Abeyweera, Sasitha C. [1 ,2 ]
Simukaitis, Matas [1 ]
Wei, Qilin [1 ]
Sun, Yugang [1 ]
机构
[1] Temple Univ, Dept Chem, 1901 North 13th St, Philadelphia, PA 19122 USA
[2] Uva Wellassa Univ, Fac Technol Studies, Dept Biosyst Technol, Badulla, Sri Lanka
来源
SMARTMAT | 2022年 / 3卷 / 01期
关键词
carbon dioxide to liquid fuels; electrical-to-chemical energy conversion; interfaced bimetallic boundaries; C-C coupling reactions; CARBON-DIOXIDE; ELECTRODE; CU; ELECTROCATALYSTS; ELECTROREDUCTION; CONVERSION;
D O I
10.1002/smm2.1096
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Selective reduction of CO2 into liquid products such as ethanol through electrochemical catalysis is promising in storing renewable energy in more deliverable chemicals and balancing the carbon footprint in the environment. However, the lack of efficient catalysts for electrochemical CO2 reduction reaction (eCO(2)RR) makes the promise challenging because the formation of C2+ alcohols requires coupling reactions between the shallow reduction intermediates and deep reduction intermediates that are usually difficult to form on uniform catalyst surfaces simultaneously with appropriate transient kinetics. Herein, we report a new strategy for synthesizing bimetallic nanostructures with high densities of interfaced Ag/Cu boundaries, which facilitate the coupling reaction of the high-oxidation-number intermediates (CO) formed on the Ag surface and the low-oxidation-number intermediates (CHx) formed on the Cu surface. The synthesis relies on the electrochemical reduction of bilayered nanoplates made of silver thiolate and copper thiolate, resulting in Ag/Cu nanostructures exposing Ag surface, Cu surface, and the Ag/Cu interfaced boundaries. Balancing the accessible surface areas of the Ag surface, Cu surface, and Ag/Cu boundaries is beneficial for maximizing the activity and selectivity of eCO(2)RR towards ethanol production. Faradaic efficiency of forming ethanol has been observed as high as about 50% using the Ag/Cu nanostructure catalyst with molar ratio n(Ag):n(Cu) of 1:1. Moreover, the promoted coupling reaction at the Ag/Cu boundaries and surface modification with thiolate anions significantly suppress the undesirable hydrogen evolution reaction, particularly at high cathodic potentials, maintaining high energy efficiency for eCO(2)RR.
引用
收藏
页码:173 / 182
页数:10
相关论文
共 41 条
[1]   Hierarchically 3D Porous Ag Nanostructures Derived from Silver Benzenethiolate Nanoboxes: Enabling CO2 Reduction with a Near-Unity Selectivity and Mass-Specific Current Density over 500 A/g [J].
Abeyweera, Sasitha C. ;
Yu, Jie ;
Perdew, John P. ;
Yan, Qimin ;
Sun, Yugang .
NANO LETTERS, 2020, 20 (04) :2806-2811
[2]   Anion replacement in silver chlorobromide nanocubes: two distinct hollowing mechanisms [J].
Abeyweera, Sasitha C. ;
Stewart, Shea ;
Sun, Yugang .
MATERIALS CHEMISTRY FRONTIERS, 2020, 4 (02) :524-531
[3]   Silver Chlorobromide Nanocubes: A Class of Reactive Templates for Synthesizing Nanoplates and Nanocages of Silver Thiolates [J].
Abeyweera, Sasitha C. ;
Sun, Yugang .
MRS ADVANCES, 2019, 4 (38-39) :2087-2094
[4]   Suppression of Hydrogen Evolution in Acidic Electrolytes by Electrochemical CO2 Reduction [J].
Bondue, Christoph J. ;
Graf, Matthias ;
Goyal, Akansha ;
Koper, Marc T. M. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2021, 143 (01) :279-285
[5]   Cu-Ag Tandem Catalysts for High-Rate CO2 Electrolysis toward Multicarbons [J].
Chen, Chubai ;
Li, Yifan ;
Yu, Sunmoon ;
Louisia, Sheena ;
Jin, Jianbo ;
Li, Mufan ;
Ross, Michael B. ;
Yang, Peidong .
JOULE, 2020, 4 (08) :1688-1699
[6]   Highly active and stable stepped Cu surface for enhanced electrochemical CO2 reduction to C2H4 [J].
Choi, Chungseok ;
Kwon, Soonho ;
Cheng, Tao ;
Xu, Mingjie ;
Tieu, Peter ;
Lee, Changsoo ;
Cai, Jin ;
Lee, Hyuck Mo ;
Pan, Xiaoqing ;
Duan, Xiangfeng ;
Goddard, William A., III ;
Huang, Yu .
NATURE CATALYSIS, 2020, 3 (10) :804-812
[7]   The Central Role of Bicarbonate in the Electrochemical Reduction of Carbon Dioxide on Gold [J].
Dunwell, Marco ;
Lu, Qi ;
Heyes, Jeffrey M. ;
Rosen, Jonathan ;
Chen, Jingguang G. ;
Yan, Yushan ;
Jiao, Feng ;
Xu, Bingjun .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2017, 139 (10) :3774-3783
[8]   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
[9]   Creating the right environment [J].
Hansen, Kentaro U. ;
Jiao, Feng .
NATURE ENERGY, 2021, 6 (11) :1005-1006
[10]   PRODUCTION OF METHANE AND ETHYLENE IN ELECTROCHEMICAL REDUCTION OF CARBON-DIOXIDE AT COPPER ELECTRODE IN AQUEOUS HYDROGENCARBONATE SOLUTION [J].
HORI, Y ;
KIKUCHI, K ;
MURATA, A ;
SUZUKI, S .
CHEMISTRY LETTERS, 1986, (06) :897-898