Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 3, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202112116
Keywords
catalytic active sites; CO2 reduction; Cu paddle wheel; electrocatalysts
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Funding
- National Natural Science Foundation of China [51872108, U20A20246]
- National Key Research and Development Program of China [2017YFA0403400]
- Fundamental Research Funds for the Central Universities [CCNU20TS006]
- China Postdoctoral Science Foundation [20201jb015]
- Hubei Postdoctoral Science Foundation [20201jb013]
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The study demonstrates that the defect-containing metal-organic framework can accelerate the electrochemical CO2 reduction reaction. By investigating the dynamic behavior of Cu-CPW, it is found to act as an active site in the deep CO2 reduction reaction.
The electrochemical reduction of CO2 to hydrocarbons involves a multistep proton-coupled electron transfer (PCET) reaction. Second coordination sphere engineering is reported to be effective in the PCET process; however, little is known about the actual catalytic active sites under realistic operating conditions. We have designed a defect-containing metal-organic framework, HKUST-1, through a facile atomized trimesic acid strategy, in which Cu atoms are modified by unsaturated carboxylate ligands, producing coordinatively unsaturated Cu paddle wheel (CU-CPW) clusters. We investigate the dynamic behavior of the CU-CPW during electrochemical reconstruction through the comprehensive analysis of in situ characterization results. It is demonstrated that Cu-2(HCOO)(3) is maintained after electrochemical reconstruction and that is behaves as an active site. Mechanistic studies reveal that CU-CPW accelerates the proton-coupled multi-electron transfer (PCMET) reaction, resulting in a deep CO2 reduction reaction.
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