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Tuning the Coordination Structure of CuNC Single Atom Catalysts for Simultaneous Electrochemical Reduction of CO2 and NO3– to Urea

Tuning the Coordination Structure of CuNC Single Atom Catalysts for Simultaneous... Closing both the carbon and nitrogen loops is a critical venture to support the establishment of the circular, net‐zero carbon economy. Although single atom catalysts (SACs) have gained interest for the electrochemical reduction reactions of both carbon dioxide (CO2RR) and nitrate (NO3RR), the structure–activity relationship for Cu SAC coordination for these reactions remains unclear and should be explored such that a fundamental understanding is developed. To this end, the role of the Cu coordination structure is investigated in dictating the activity and selectivity for the CO2RR and NO3RR. In agreement with the density functional theory calculations, it is revealed that Cu‐N4 sites exhibit higher intrinsic activity toward the CO2RR, whilst both Cu‐N4 and Cu‐N4−x‐Cx sites are active toward the NO3RR. Leveraging these findings, CO2RR and NO3RR are coupled for the formation of urea on Cu SACs, revealing the importance of *COOH binding as a critical parameter determining the catalytic activity for urea production. To the best of the authors’ knowledge, this is the first report employing SACs for electrochemical urea synthesis from CO2RR and NO3RR, which achieves a Faradaic efficiency of 28% for urea production with a current density of −27 mA cm–2 at −0.9 V versus the reversible hydrogen electrode. http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png Advanced Energy Materials Wiley

Tuning the Coordination Structure of CuNC Single Atom Catalysts for Simultaneous Electrochemical Reduction of CO2 and NO3– to Urea

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Publisher
Wiley
Copyright
© 2022 Wiley‐VCH GmbH
ISSN
1614-6832
eISSN
1614-6840
DOI
10.1002/aenm.202201500
Publisher site
See Article on Publisher Site

Abstract

Closing both the carbon and nitrogen loops is a critical venture to support the establishment of the circular, net‐zero carbon economy. Although single atom catalysts (SACs) have gained interest for the electrochemical reduction reactions of both carbon dioxide (CO2RR) and nitrate (NO3RR), the structure–activity relationship for Cu SAC coordination for these reactions remains unclear and should be explored such that a fundamental understanding is developed. To this end, the role of the Cu coordination structure is investigated in dictating the activity and selectivity for the CO2RR and NO3RR. In agreement with the density functional theory calculations, it is revealed that Cu‐N4 sites exhibit higher intrinsic activity toward the CO2RR, whilst both Cu‐N4 and Cu‐N4−x‐Cx sites are active toward the NO3RR. Leveraging these findings, CO2RR and NO3RR are coupled for the formation of urea on Cu SACs, revealing the importance of *COOH binding as a critical parameter determining the catalytic activity for urea production. To the best of the authors’ knowledge, this is the first report employing SACs for electrochemical urea synthesis from CO2RR and NO3RR, which achieves a Faradaic efficiency of 28% for urea production with a current density of −27 mA cm–2 at −0.9 V versus the reversible hydrogen electrode.

Journal

Advanced Energy Materials – Wiley

Published: Aug 1, 2022

Keywords: CO 2 reduction; Cu single atom; power to X, urea

References

  • The Role of the Chemical Sciences in Finding Alternatives to Critical Resources
    Friedman, D.; Masciangioli, T.; Olson, S.