Affiliation:
1. Department of Chemistry City University of Hong Kong Kowloon Hong Kong SAR 999077 P. R. China
2. Laboratory of Theoretical and Computational Chemistry Institute of Theoretical Chemistry Jilin University Changchun 130012 P. R. China
3. Department of Chemical Engineering and Biotechnology University of Cambridge Cambridge CB2 3RA UK
Abstract
AbstractMolecular catalysts represent an exceptional class of materials in the realm of electrochemical carbon dioxide reduction (CO2RR), offering distinct advantages owing to their adaptable structure, which enables precise control of electronic configurations and outstanding performance in CO2RR. This study introduces an innovative approach to heterogeneous electrochemical CO2RR in an aqueous environment, utilizing a newly synthesized N4‐macrocyclic cobalt complex generated through a dimerization coupling reaction. By incorporating the quaterpyridine moiety, this cobalt complex exhibits the capability to catalyze CO2RR at low overpotentials and reaches near‐unity CO production across a wide potential range, as verified by the online mass spectrometry and in situ attenuated total reflectance‐Fourier transform infrared spectroscopy. Comprehensive computational models demonstrate the superiority of utilizing quarterpyridine moiety in mediating CO2 conversion compared to the counterpart. This work not only propels the field of electrochemical CO2RR but also underscores the promising potential of cobalt complexes featuring quaterpyridine moieties in advancing sustainable CO2 conversion technologies within aqueous environments.
Funder
City University of Hong Kong
National Research Foundation Singapore
Innovation and Technology Commission - Hong Kong