Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 141, Issue 32, Pages 12717-12723Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.9b04907
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Funding
- National Natural Science Foundation of China [21571131]
- Natural Science Foundation of Guangdong Province [2017A040405066]
- Shenzhen Government's Plan of Science and Technology [JCYJ20160308104704791, JCYJ20170818091657056]
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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.
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