期刊
NATURE NANOTECHNOLOGY
卷 16, 期 12, 页码 1386-U94出版社
NATURE PORTFOLIO
DOI: 10.1038/s41565-021-00974-5
关键词
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资金
- University of Electronic Science and Technology of China (UESTC) [A1098531023601264]
- NSFC [22102018, 52171201, U19A2015, 91845103, 22005291]
- National Key Research and Development Program of China [2019YFA0405600]
- National Science Fund for Distinguished Young Scholars [21925204]
- Fundamental Research Funds for the Central Universities
- Provincial Key Research and Development Program of Anhui [202004a05020074]
- DNL Cooperation Fund, CAS [DNL202003]
- USTC Research Funds of the Double First-Class Initiative [YD2340002002]
- Ministry of Science and Technology of China [2018YFA0704503]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB36030200]
- LiaoNing Revitalization Talents Program [XLYC1907099]
- China Postdoctoral Science Foundation [2019TQ0300, 2020M671890]
- Beijing Outstanding Young Scientist Program [BJJWZYJH01201914430039]
The single-atom Pb-alloyed Cu catalyst (Pb1Cu) efficiently converts CO2 into formic acid with high selectivity and activity, offering the potential to increase productivity.
Converting CO2 emissions, powered by renewable electricity, to produce fuels and chemicals provides an elegant route towards a carbon-neutral energy cycle. Progress in the understanding and synthesis of Cu catalysts has spurred the explosive development of electrochemical CO2 reduction (CO2RR) technology to produce hydrocarbons and oxygenates; however, Cu, as the predominant catalyst, often exhibits limited selectivity and activity towards a specific product, leading to low productivity and substantial post-reaction purification. Here, we present a single-atom Pb-alloyed Cu catalyst (Pb1Cu) that can exclusively (similar to 96% Faradaic efficiency) convert CO2 into formate with high activity in excess of 1 A cm(-2). The Pb1Cu electrocatalyst converts CO2 into formate on the modulated Cu sites rather than on the isolated Pb. In situ spectroscopic evidence and theoretical calculations revealed that the activated Cu sites of the Pb1Cu catalyst regulate the first protonation step of the CO2RR and divert the CO2RR towards a HCOO* path rather than a COOH* path, thus thwarting the possibility of other products. We further showcase the continuous production of a pure formic acid solution at 100 mA cm(-2) over 180 h using a solid electrolyte reactor and Pb1Cu.
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