Predesign of Catalytically Active Sites via Stable Coordination Cluster Model System for Electroreduction of CO2 to Ethylene

Purposefully designing the well‐defined catalysts for the selective electroreduction of CO2 to C2H4 is an extremely important but challenging work. In this work, three crystalline trinuclear copper clusters (Cu3‐X, X=Cl−, Br−, NO3−) have been designed, containing three active Cu sites with the ident...

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Published inAngewandte Chemie International Edition Vol. 60; no. 50; pp. 26210 - 26217
Main Authors Lu, Yun‐Feng, Dong, Long‐Zhang, Liu, Jiang, Yang, Ru‐Xin, Liu, Jing‐Jing, Zhang, Yu, Zhang, Lei, Wang, Yi‐Rong, Li, Shun‐Li, Lan, Ya‐Qian
Format Journal Article
LanguageEnglish
Published Weinheim Wiley Subscription Services, Inc 06.12.2021
EditionInternational ed. in English
Subjects
active sites
Anions
Carbon dioxide
Catalysts
Chemical reduction
CO2 reduction
Coordination
Copper
Coupling (molecular)
C−C coupling
electrocatalysis
Electrowinning
Intermediates
molecular catalysts
Molecular structure
Selectivity
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Summary:Purposefully designing the well‐defined catalysts for the selective electroreduction of CO2 to C2H4 is an extremely important but challenging work. In this work, three crystalline trinuclear copper clusters (Cu3‐X, X=Cl−, Br−, NO3−) have been designed, containing three active Cu sites with the identical coordination environment and appropriate spatial distance, delivering high selectivity for the electrocatalytic reduction of CO2 to C2H4. The highest faradaic efficiency of Cu3‐X for CO2‐to‐C2H4 conversion can be adjusted from 31.90 % to 55.01 % by simply replacing the counter anions (NO3−, Cl−, Br−). The DFT calculation results verify that Cu3‐X can facilitate the C−C coupling of identical *CHO intermediates, subsequently forming molecular symmetrical C2H4 product. This work provides an important molecular model system and a new design perspective for electroreduction of CO2 to C2 products with symmetrical molecular structure. A molecular model catalyst system (Cu3‐X) with predesigned catalytically active sites has been constructed to achieve the selective electroreduction of CO2 to C2H4. The active Cu sites display an appropriate spatial distance, resulting in high faradaic efficiencies.
Bibliography:These authors contributed equally to this work.
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ISSN:1433-7851
1521-3773
1521-3773
DOI:10.1002/anie.202111265