CO2 Electroreduction to Hydrocarbons on Carbon-Supported Cu Nanoparticles

被引:278
作者
Baturina, Olga A. [1 ]
Lu, Qin [1 ]
Padilla, Monica A. [3 ]
Xin, Le [4 ]
Li, Wenzhen [4 ]
Serov, Alexey [3 ]
Artyushkova, Kateryna [3 ]
Atanassov, Plamen [3 ]
Xu, Feng [5 ,6 ]
Epshteyn, Albert [1 ]
Brintlinger, Todd [2 ]
Schuette, Mike [7 ]
Collins, Greg E. [1 ]
机构
[1] Naval Res Lab, Div Chem, Washington, DC 20375 USA
[2] Naval Res Lab, Mat Sci & Technol Div, Washington, DC 20375 USA
[3] Univ New Mexico, Dept Chem & Nucl Engn, Albuquerque, NM 87131 USA
[4] Michigan Technol Univ, Dept Chem & Biol Engn, Houghton, MI 49931 USA
[5] Univ Oxford, Dept Chem, Wolfson Catalysis Ctr, Oxford OX1 3QR, England
[6] Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
[7] Sotera Inc, Herndon, VA 20171 USA
来源
ACS CATALYSIS | 2014年 / 4卷 / 10期
基金
美国国家科学基金会;
关键词
CO2; electroreduction; rotating disk electrode; Faradaic efficiency; copper nanoparticles; electrocatalytic activity; hydrocarbons; methane; ethylene; SINGLE-CRYSTAL ELECTRODES; ELECTROCHEMICAL REDUCTION; COPPER ELECTRODE; ELECTROCATALYTIC CONVERSION; AMBIENT-TEMPERATURE; DIOXIDE REDUCTION; AQUEOUS-SOLUTIONS; SURFACE; OXIDE; SELECTIVITY;
D O I
10.1021/cs500537y
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
Activities of Cu nanopartides supported on carbon black (VC), single-wall carbon nanotubes (SWNTs), and Ketjen Black (KB) toward CO2 electroreduction to hydrocarbons (CH4, C2H2, C2H4, and C2H6) are evaluated using a sealed rotating disk electrode (RDE) setup coupled to a gas clu-omatograph (GC). Thin films of supported Cu catalysts are deposited on RDE tips following a procedure well-established in the fuel cell community. Lead (Pb) underpotential deposition (UPD) is used to determine the electrochemical surface area (ECSA) of thin films of 40 wt % Cu/VC, 20 wt % Cu/SWNT, 50 wt % Cu/KB, and commercial 20 wt % Cu/VC catalysts on glassy carbon electrodes. Faradaic efficiencies of four carbon-supported Cu catalysts toward CO2 electroreduction to hydrocarbons are compared to that of electrodeposited smooth Cu films. For all the catalysts studied, the only hydrocarbons detected by GC are CH4 and C2H4. The Cu nanoparticles are found to be more active toward C2H4 generation versus electrodeposited smooth copper films. For the supported Cu nanocatalysts, the ratio of C2H4/CH4 Faradaic efficiencies is believed to be a function of particle size, as higher ratios are observed for smaller Cu nanoparticles. This is likely due to an increase in the fraction of under-coordinated sites, such as corners, edges, and defects, as the nanopartides become smaller.
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页码:3682 / 3695
页数:14
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