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Scalable Production of Efficient Single-Atom Copper Decorated Carbon Membranes for CO₂ Electroreduction to Methanol

Yang, Hengpan, Wu, Yu, Li, Guodong, Lin, Qing, Hu, Qi, Zhang, Qianling, Liu, Jianhong, He, Chuanxin
Journal of the American Chemical Society 2019 v.141 no.32 pp. 12717-12723
aqueous solutions, carbon, carbon dioxide, carbon monoxide, carbon nanofibers, catalysts, catalytic activity, cathodes, copper, electrochemistry, energy, high-value products, hydrocarbons, mechanical properties, methanol
Electrocatalytic reduction reaction of CO₂ (CO₂RR) is an effective way to mitigate energy and environmental issues. However, very limited catalysts are capable of converting CO₂ resources into high-value products such as hydrocarbons or alcohols. Herein, we first propose a facile strategy for the large-scale synthesis of isolated Cu decorated through-hole carbon nanofibers (CuSAs/TCNFs). This CuSAs/TCNFs membrane has excellent mechanical properties and can be directly used as cathode for CO₂RR, which could generate nearly pure methanol with 44% Faradaic efficiency in liquid phase. The self-supporting and through-hole structure of CuSAs/TCNFs greatly reduces the embedded metal atoms and produces abundant efficient Cu single atoms, which could actually participate in CO₂RR, eventually causing −93 mA cm–² partial current density for C1 products and more than 50 h stability in aqueous solution. According to DFT calculations, Cu single atoms possess a relatively higher binding energy for *CO intermediate. Therefore, *CO could be further reduced to products like methanol, instead of being easily released from the catalyst surface as CO product. This report may benefit the design of efficient and high-yield single-atom catalysts for other electrocatalytic reactions.