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Nano Research 2023, 16(7): 8987-8995 https://doi.org/10.1007/s12274-023-5640-z
Research Article | Issue | Published: 25 April 2023

Ultrastable nickel single-atom catalysts with high activity and selectivity for electrocatalytic CO2 methanation

Show Author's Information Ling-Chan Tian1,  Jin-Nian Hu1,  Yang Meng1,  Jin-Xia Liang1( ),  Chun Zhu1,2( ),  Jun Li2,3
School of Chemistry and Chemical Engineering, Guizhou University, Guiyang 550025, China
Department of Chemistry and Guangdong Provincial Key Laboratory of Catalytic Chemistry, Southern University of Science and Technology, Shenzhen 518055, China
Department of Chemistry and Engineering Research Center of Advanced Rare-Earth Materials of Ministry of Education, Tsinghua University, Beijing 100084, China
Keywords:
density functional theory, electrocatalysis, CO2 reduction, single atom catalyst, metal–organic framework
Topics:
Electrocatalysis
Cite this article:
Tian L-C, Hu J-N, Meng Y, et al. Ultrastable nickel single-atom catalysts with high activity and selectivity for electrocatalytic CO2 methanation. Nano Research, 2023, 16(7): 8987-8995. https://doi.org/10.1007/s12274-023-5640-z
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Abstract Full text Electronic supplementary material About this article

Electrochemical conversion of CO2 into valuable hydrocarbon fuel is one of the key steps in solving carbon emission and energy issue. Herein, we report a non-noble metal catalyst, nickel single-atom catalyst (SAC) of Ni1/UiO-66-NH2, with high stability and selectivity for electrochemical reduction of CO2 to CH4. Based on ab initio molecular dynamics (AIMD) simulations, the CO2 molecule is at first reduced into CO2− when stably adsorbed on a Ni single atom with the bidentate coordination mode. To evaluate its activity and selectivity for electrocatalytic reduction of CO2 to different products (HCOOH, CO, CH3OH, and CH4) on Ni1/UiO-66-NH2, we have used density functional theory (DFT) to study different reaction pathways. The results show that CH4 is generated preferentially on Ni1/UiO-66-NH2 and the calculated limiting potential is as low as −0.24 V. Moreover, the competitive hydrogen evolution reaction is unfavorable at the activation site of Ni1/UiO-66-NH2 owing to the higher limiting potential of −0.56 V. Furthermore, the change of Ni single atom valence state plays an important role in promoting CO2 reduction to CH4. This work provides a theoretical foundation for further experimental studies and practical applications of metal–organic framework (UiO-66)-based SAC electrocatalysts with high activity and selectivity for the CO2 reduction reaction.


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About this article

Ultrastable nickel single-atom catalysts with high activity and selectivity for electrocatalytic CO2 methanation

Show Author's information Ling-Chan Tian1, Jin-Nian Hu1, Yang Meng1, Jin-Xia Liang1( ), Chun Zhu1,2( ), Jun Li2,3
School of Chemistry and Chemical Engineering, Guizhou University, Guiyang 550025, China
Department of Chemistry and Guangdong Provincial Key Laboratory of Catalytic Chemistry, Southern University of Science and Technology, Shenzhen 518055, China
Department of Chemistry and Engineering Research Center of Advanced Rare-Earth Materials of Ministry of Education, Tsinghua University, Beijing 100084, China

Abstract

Electrochemical conversion of CO2 into valuable hydrocarbon fuel is one of the key steps in solving carbon emission and energy issue. Herein, we report a non-noble metal catalyst, nickel single-atom catalyst (SAC) of Ni1/UiO-66-NH2, with high stability and selectivity for electrochemical reduction of CO2 to CH4. Based on ab initio molecular dynamics (AIMD) simulations, the CO2 molecule is at first reduced into CO2− when stably adsorbed on a Ni single atom with the bidentate coordination mode. To evaluate its activity and selectivity for electrocatalytic reduction of CO2 to different products (HCOOH, CO, CH3OH, and CH4) on Ni1/UiO-66-NH2, we have used density functional theory (DFT) to study different reaction pathways. The results show that CH4 is generated preferentially on Ni1/UiO-66-NH2 and the calculated limiting potential is as low as −0.24 V. Moreover, the competitive hydrogen evolution reaction is unfavorable at the activation site of Ni1/UiO-66-NH2 owing to the higher limiting potential of −0.56 V. Furthermore, the change of Ni single atom valence state plays an important role in promoting CO2 reduction to CH4. This work provides a theoretical foundation for further experimental studies and practical applications of metal–organic framework (UiO-66)-based SAC electrocatalysts with high activity and selectivity for the CO2 reduction reaction.

Keywords: density functional theory, electrocatalysis, CO2 reduction, single atom catalyst, metal–organic framework

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Publication history
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Acknowledgements

Publication history

Received: 10 January 2023
Revised: 27 February 2023
Accepted: 02 March 2023
Published: 25 April 2023
Issue date: July 2023

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was supported by the National Key Research and Development Project (Nos. 2022YFA1503900 and 2022YFA1503000), the National Natural Science Foundation of China (Nos. 22033005 and 21963005), the Natural Science Special Foundation of Guizhou University (No. 202140), and the Guangdong Provincial Key Laboratory of Catalysis (No. 2020B121201002). The calculations were performed using supercomputers at the Center for Computational Science and Engineering of SUSTech and Shanghai Supercomputing Center.

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