CO2 Electroreduction to Hydrocarbons on Carbon-Supported Cu Nanoparticles

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• 作者：Olga A. Baturina ; Qin Lu ; Monica A. Padilla ; Le Xin ; Wenzhen Li ; Alexey Serov ; Kateryna Artyushkova ; Plamen Atanassov ; Feng Xu ; Albert Epshteyn ; Todd Brintlinger ; Mike Schuette ; Greg E. Collins
• 刊名：ACS Catalysis
• 出版年：2014
• 出版时间：October 3, 2014
• 年：2014
• 卷：4
• 期：10
• 页码：3682-3695
• 全文大小：757K
• ISSN：2155-5435

文摘

Activities of Cu nanoparticles 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 chromatograph (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 nanoparticles become smaller.

Keywords:

CO₂ electroreduction; rotating disk electrode; Faradaic efficiency; copper nanoparticles; electrocatalytic activity; hydrocarbons; methane; ethylene