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Nano Research 2024, 17(4): 3413-3422 https://doi.org/10.1007/s12274-023-6140-x
Research Article | Issue | Published: 11 November 2023

Theoretical screening of cooperative N-bridged dual-atom sites for efficient electrocatalytic nitrogen reduction with remolding insight

Show Author's Information Huimei Chen,§,  Yan Yang,§,  Chi Jiao,  Zhiwen Zhuo( ),  Junjie Mao( ),  Yan Liu( )
Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu 241002, China

§ Huimei Chen and Yan Yang contributed equally to this work.

Keywords:
hydrogen evolution reaction, density functional theory calculations, nitrogen reduction, high-throughput screening, dual-atom catalysts
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Chen H, Yang Y, Jiao C, et al. Theoretical screening of cooperative N-bridged dual-atom sites for efficient electrocatalytic nitrogen reduction with remolding insight. Nano Research, 2024, 17(4): 3413-3422. https://doi.org/10.1007/s12274-023-6140-x
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Abstract Full text Electronic supplementary material About this article

The electrocatalytic nitrogen reduction reaction (e-NRR) is a promising alternative method for the Haber–Bosch process. However, it still faces many challenges in searching for high activity, stability, and selectivity catalysts and ascertaining the catalytic mechanism with complete insight. Here, a series of graphene-based N-bridged dual-atom catalysts (M1-N-M2/NC) are systematically investigated via first-principle calculation and a high-throughput screening strategy. The result unveils that N2 adsorption on M1-N-M2/NC in bridge-on adsorption mode can effectively break the scaling relationship on single-atom catalysts (SACs). Moreover, V-N-Ru/NC and V-N-Os/NC are systematically screened out as promising e-NRR catalysts, with extremely low limiting potentials of −0.20 and −0.18 V, respectively. Furthermore, the adsorption site competition between *N2 and *H, as well as the competitive twin reactions of hydrogen evolution reaction (HER) on intermediates (NnHm) during the e-NRR process, is systematically evaluated to form a remodeling insight for the reactions in mechanism, and the e-NRR of new proposed dual-atom catalysts (DACs) is strategically optimized for its high-efficiency performance potential via our remolding insight in e-NRR mechanism. This work provides new ideas and insights for the design and mechanism of e-NRR catalysts and an effective strategy for rapidly screening highly efficient e-NRR catalysts.


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Abstract
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Electronic supplementary material
About this article

Theoretical screening of cooperative N-bridged dual-atom sites for efficient electrocatalytic nitrogen reduction with remolding insight

Show Author's information Huimei Chen,§, Yan Yang,§, Chi Jiao, Zhiwen Zhuo( ), Junjie Mao( ), Yan Liu( )
Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu 241002, China

§ Huimei Chen and Yan Yang contributed equally to this work.

Abstract

The electrocatalytic nitrogen reduction reaction (e-NRR) is a promising alternative method for the Haber–Bosch process. However, it still faces many challenges in searching for high activity, stability, and selectivity catalysts and ascertaining the catalytic mechanism with complete insight. Here, a series of graphene-based N-bridged dual-atom catalysts (M1-N-M2/NC) are systematically investigated via first-principle calculation and a high-throughput screening strategy. The result unveils that N2 adsorption on M1-N-M2/NC in bridge-on adsorption mode can effectively break the scaling relationship on single-atom catalysts (SACs). Moreover, V-N-Ru/NC and V-N-Os/NC are systematically screened out as promising e-NRR catalysts, with extremely low limiting potentials of −0.20 and −0.18 V, respectively. Furthermore, the adsorption site competition between *N2 and *H, as well as the competitive twin reactions of hydrogen evolution reaction (HER) on intermediates (NnHm) during the e-NRR process, is systematically evaluated to form a remodeling insight for the reactions in mechanism, and the e-NRR of new proposed dual-atom catalysts (DACs) is strategically optimized for its high-efficiency performance potential via our remolding insight in e-NRR mechanism. This work provides new ideas and insights for the design and mechanism of e-NRR catalysts and an effective strategy for rapidly screening highly efficient e-NRR catalysts.

Keywords: hydrogen evolution reaction, density functional theory calculations, nitrogen reduction, high-throughput screening, dual-atom catalysts

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Publication history
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Acknowledgements

Publication history

Received: 19 July 2023
Revised: 28 August 2023
Accepted: 29 August 2023
Published: 11 November 2023
Issue date: April 2024

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (No. 21971002) and the Natural Science Foundation of Anhui province (Nos. 2008085QB81 and 2208085QA11). The numerical calculations in this paper have been done on Hefei advanced computing center.

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