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Superoxide-derived Selective Reduction of CO2 to CO at Low Overpotentials in Ionic Liquid

Faculty #28
Discipline: Chemistry & Chemical Sciences
Subcategory: STEM Research
- Xavier University of Louisiana
Co-Author(s): Zhongyuan Huang, Kevin E. Riley and Guangdi Wang, Xavier University of Louisiana , New Orleans, LA; Aayush Gupta and Petr Král, University of Illinois, Chicago , Chicago, IL; Douglas B. Chrisey, Tulane University, New Orleans, LA



Electroreduction of CO2 using high selective and efficient ways is the key point of CO2 utilization. Here we reported the electrocatalytic approach that can be used for the rational design of CO2 reduction system with potentially using any electrodes in aerobic environments. In this system, CO2 reduction displayed at very low over-potential, >90% faradic efficiency and near 100% of carbon selectivity to CO. This approach was initiated from the superoxide radicals (O2.-) electrochemical generation, and further CO2 was efficiently activated through the CO2 adducts N-heterocyclic carbenes (NHCs) in 1-Butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (Bmim NTf2) ionic liquid. Electrochemical and computational results suggested a ECE mechanism, in which O2.- efficiently transform Bmim cations to N-heterocyclic carbine (NHC) structure, and which further activate CO2 with NHC-CO2. This work offers a green approach for CO2 reduction supply under simplicity and mild conditions, which have potential application in a broad range of molecular-material platforms and catalytic systems, and also O2 involved biological processes.

Funder Acknowledgement(s): National Science Foundation (Grant HRD 1700429); NIMHD-RCMI grant number 5G12MD007595; NIGMS-BUILD grant number 8UL1GM118967

Faculty Advisor: None Listed,

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This material is based upon work supported by the National Science Foundation (NSF) under Grant No. DUE-1930047. Any opinions, findings, interpretations, conclusions or recommendations expressed in this material are those of its authors and do not represent the views of the AAAS Board of Directors, the Council of AAAS, AAAS’ membership or the National Science Foundation.

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