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Interatomic Electronegativity Offset Dictates Selectivity When Catalyzing the CO2 Reduction Reaction

Interatomic Electronegativity Offset Dictates Selectivity When Catalyzing the CO2 Reduction Reaction Achieving efficient efficiency and selectivity for the electroreduction of CO2 to value‐added feedstocks has been challenging, due to the thermodynamic stability of CO2 molecules and the competing hydrogen evolution reaction. Herein, a dual‐single‐atom catalyst consisting of atomically dispersed CuN4 and NiN4 bimetal sites is synthesized with electrospun carbon nanofibers (CuNi‐DSA/CNFs). Theoretical and experimental studies reveal the strong electron interactions induced by the electronegativity offset between the Cu and Ni atoms. The delicately averaged and compensated electronic structures result in an offset effect that optimizes the adsorption strength of the *COOH intermediate and boosts the CO2 reduction reaction (CO2RR) kinetics, notably promoting the intrinsic activity and selectivity of the catalyst. The CuNi‐DSA/CNFs catalyst exhibits an outstanding FECO of 99.6% across a broad potential window of −0.78– −1.18 V (vs the reversible hydrogen electrode), a high turnover frequency of 2870 h–1, and excellent durability (25 h). Furthermore, an aqueous Zn‐CO2 battery for CO2 power conversion is constructed. This atomic‐level electronegativity offset of the dual‐atom structures provides an appealing direction to develop advanced electrocatalysts for the CO2RR. http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png Advanced Energy Materials Wiley

Interatomic Electronegativity Offset Dictates Selectivity When Catalyzing the CO2 Reduction Reaction

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References (34)

Publisher
Wiley
Copyright
© 2022 Wiley‐VCH GmbH
ISSN
1614-6832
eISSN
1614-6840
DOI
10.1002/aenm.202200579
Publisher site
See Article on Publisher Site

Abstract

Achieving efficient efficiency and selectivity for the electroreduction of CO2 to value‐added feedstocks has been challenging, due to the thermodynamic stability of CO2 molecules and the competing hydrogen evolution reaction. Herein, a dual‐single‐atom catalyst consisting of atomically dispersed CuN4 and NiN4 bimetal sites is synthesized with electrospun carbon nanofibers (CuNi‐DSA/CNFs). Theoretical and experimental studies reveal the strong electron interactions induced by the electronegativity offset between the Cu and Ni atoms. The delicately averaged and compensated electronic structures result in an offset effect that optimizes the adsorption strength of the *COOH intermediate and boosts the CO2 reduction reaction (CO2RR) kinetics, notably promoting the intrinsic activity and selectivity of the catalyst. The CuNi‐DSA/CNFs catalyst exhibits an outstanding FECO of 99.6% across a broad potential window of −0.78– −1.18 V (vs the reversible hydrogen electrode), a high turnover frequency of 2870 h–1, and excellent durability (25 h). Furthermore, an aqueous Zn‐CO2 battery for CO2 power conversion is constructed. This atomic‐level electronegativity offset of the dual‐atom structures provides an appealing direction to develop advanced electrocatalysts for the CO2RR.

Journal

Advanced Energy MaterialsWiley

Published: Jul 1, 2022

Keywords: CO 2 electroreduction reaction; dual single atoms; electrospun nanofibers; interatomic electronegativity compensation

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