Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 38, Pages 20803-20810Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202105263
Keywords
carbon dioxide; electrocatalysis; green chemistry; ionic liquids; single-atom catalysts
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Funding
- National Key Research and Development Program of China [2017YFA0403101, 2017YFA0403003, 2017YFA0403102]
- National Natural Science Foundation of China [21890761, 21733011]
- Chinese Academy of Sciences [QYZDY-SSW-SLH013]
- Beijing Municipal Science AMP
- Technology Commission [Z191100007219009]
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Guided by first-principles calculations, it was discovered that Cd single-atom catalysts have excellent performance in activating CO2, and the introduction of axial coordination structure can further decrease the free energy barrier of CO2 reduction while suppressing the hydrogen evolution reaction. The designed and synthesized novel Cd SAC showed outstanding performance in CO2 electroreduction to CO, achieving a high faradaic efficiency and turnover frequency. This work serves as a successful example of designing highly efficient catalysts guided by theoretical calculations.
Guided by first-principles calculations, it was found that Cd single-atom catalysts (SACs) have excellent performance in activating CO2, and the introduction of axial coordination structure to Cd SACs cannot only further decrease the free energy barrier of CO2 reduction, but also suppress the hydrogen evolution reaction (HER). Based on the above discovery, we designed and synthesized a novel Cd SAC that comprises an optimized CdN4S1 moiety incorporated in a carbon matrix. It was shown that the catalyst exhibited outstanding performance in CO2 electroreduction to CO. The faradaic efficiency (FE) of CO could reach up to 99.7 % with a current density of 182.2 mA cm(-2) in a H-type electrolysis cell, and the turnover frequency (TOF) value could achieve 73000 h(-1), which was much higher than that reported to date. This work shows a successful example of how to design highly efficient catalysts guided by theoretical calculations.
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