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Nano Research 2023, 16(7): 8800-8808 https://doi.org/10.1007/s12274-023-5515-3
Research Article | Issue | Published: 20 April 2023

Highly efficient hydrogen production from methanol by single nickel atoms anchored on defective boron nitride nanosheet

Show Author's Information Shengshu Yang1,2,  Fang Zhang3,  Haifa Qiu4,  Ming Yang4,  Fengjuan Qin5,  Hao Tang5,  Wenxing Chen5,  Zhengang Liu1,2( )
Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
National Engineering Laboratory for VOCs Pollution Control Material & Technology, University of Chinese Academy of Sciences, Beijing 101408, China
Analytical and Testing Center, Beijing Institute of Technology, Beijing 100081, China
Department of Applied Physics, the Hong Kong Polytechnic University, Hong Kong 999077, China
Energy & Catalysis Center, School of Materials Science & Engineering, Beijing Institute of Technology, Beijing 100081, China
Keywords:
boron nitride, single-atom catalyst, coordination environment, hydrogen production, liquid organic hydrogen carriers
Topics:
Catalysis
Cite this article:
Yang S, Zhang F, Qiu H, et al. Highly efficient hydrogen production from methanol by single nickel atoms anchored on defective boron nitride nanosheet. Nano Research, 2023, 16(7): 8800-8808. https://doi.org/10.1007/s12274-023-5515-3
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Abstract Full text Electronic supplementary material About this article

Exploiting inexpensive and effective nickel-based catalysts that produce hydrogen from liquid organic hydrogen carriers (LOHCs) is crucial to alleviating the global energy and environmental crisis. In this study, we report a rational strategy that can realize atomically dispersed Ni atoms anchored on vacancy-abundant boron nitride nanosheets (Ni1/h-BNNS) with high specific surface area (up to 622 m2·g−1) and abundant hydroxyl groups for high efficient hydrogen production. Methanol dehydrogenation results show an excellent hydrogen production performance catalyzed by this Ni1/h-BNNS, as evidenced by a remarkably high H2 yield rate (1684.23 mol·molNi−1·h−1), nearly 100% selectivity toward hydrogen and CO, and high anti-coking performance. Density functional theory (DFT) calculations reveal that the outstanding catalytic performance of Ni1/h-BNNS primarily originates from the unique coordinated environment of atomically dispersed Ni (Ni-B2O2) and the synergistic interaction between Ni single atoms and the h-BNNS support. Specifically, the coordinated O atoms play a decisive role in promoting the activity of Ni, and the neighboring B sites significantly decrease the energy barriers for the adsorption of key intermediates of methanol dehydrogenation. This study offers a novel strategy for developing high-performance and stable single-atom Ni catalysts by precisely controlling single-atom sites on h-BN support for sustainable hydrogen production.


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Electronic supplementary material
About this article

Highly efficient hydrogen production from methanol by single nickel atoms anchored on defective boron nitride nanosheet

Show Author's information Shengshu Yang1,2, Fang Zhang3, Haifa Qiu4, Ming Yang4, Fengjuan Qin5, Hao Tang5, Wenxing Chen5, Zhengang Liu1,2( )
Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
National Engineering Laboratory for VOCs Pollution Control Material & Technology, University of Chinese Academy of Sciences, Beijing 101408, China
Analytical and Testing Center, Beijing Institute of Technology, Beijing 100081, China
Department of Applied Physics, the Hong Kong Polytechnic University, Hong Kong 999077, China
Energy & Catalysis Center, School of Materials Science & Engineering, Beijing Institute of Technology, Beijing 100081, China

Abstract

Exploiting inexpensive and effective nickel-based catalysts that produce hydrogen from liquid organic hydrogen carriers (LOHCs) is crucial to alleviating the global energy and environmental crisis. In this study, we report a rational strategy that can realize atomically dispersed Ni atoms anchored on vacancy-abundant boron nitride nanosheets (Ni1/h-BNNS) with high specific surface area (up to 622 m2·g−1) and abundant hydroxyl groups for high efficient hydrogen production. Methanol dehydrogenation results show an excellent hydrogen production performance catalyzed by this Ni1/h-BNNS, as evidenced by a remarkably high H2 yield rate (1684.23 mol·molNi−1·h−1), nearly 100% selectivity toward hydrogen and CO, and high anti-coking performance. Density functional theory (DFT) calculations reveal that the outstanding catalytic performance of Ni1/h-BNNS primarily originates from the unique coordinated environment of atomically dispersed Ni (Ni-B2O2) and the synergistic interaction between Ni single atoms and the h-BNNS support. Specifically, the coordinated O atoms play a decisive role in promoting the activity of Ni, and the neighboring B sites significantly decrease the energy barriers for the adsorption of key intermediates of methanol dehydrogenation. This study offers a novel strategy for developing high-performance and stable single-atom Ni catalysts by precisely controlling single-atom sites on h-BN support for sustainable hydrogen production.

Keywords: boron nitride, single-atom catalyst, coordination environment, hydrogen production, liquid organic hydrogen carriers

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Publication history
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Acknowledgements

Publication history

Received: 02 November 2022
Revised: 27 December 2022
Accepted: 18 January 2023
Published: 20 April 2023
Issue date: July 2023

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was funded by the Shandong Province Major Scientific and Technological Innovation Project (No. 2021CXGC010803) and the National Natural Science Foundation of China (No. 21876188). M. Y. acknowledges National Research Foundation Competitive Research Programs (No. NRFCRP24-2020-0002). M. Y. acknowledges the funding support (project ID: 1-BE47, ZE0C, ZE2F, and ZE2X) from the Hong Kong Polytechnic University. We acknowledge the Centre for Advanced 2D Materials and Graphene Research at the National University of Singapore and the National Supercomputing Centre Singapore for providing computing resources. We thank H. Q. and M. Y. for their efforts in DFT computations.

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