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Nano Research 2024, 17(5): 3827-3834 https://doi.org/10.1007/s12274-023-6334-2
Research Article | Issue | Published: 12 December 2023

Design of bifunctional single-atom catalysts NiSA/ZIF-300 for CO2 conversion by ligand regulation strategy

Show Author's Information Wengang Fu1,§,  Yapei Yun1,§,  Hongting Sheng1( ),  Xiaokang Liu3,  Tao Ding3,  Shuxian Hu4,  Tao Yao3,  Binghui Ge1,  Yuanxin Du1,  Didier Astruc2( ),  Manzhou Zhu1,5( )
Department of Chemistry and Centre for Atomic Engineering of Advanced Materials, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, College of Materials Science and Engineering, Institutes of Physical Science and Information Technology and Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized Materials, Anhui University, Hefei 230601, China
Université de Bordeaux, ISM, UMR CNRS N°5255, 351 Cours de La Libération, 33405 Talence Cedex, France
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230026, China
Department of Physics, University of Science and Technology Beijing, Beijing 100083, China
Anhui Tongyuan Environment Energy Saving Co., Ltd, Hefei 230041, China

§ Wengang Fu and Yapei Yun contributed equally to this work.

Keywords:
catalyst, CO2 conversion, cycloaddition, single atom, bifunctional
Topics:
Nanocatalysts
Cite this article:
Fu W, Yun Y, Sheng H, et al. Design of bifunctional single-atom catalysts NiSA/ZIF-300 for CO2 conversion by ligand regulation strategy. Nano Research, 2024, 17(5): 3827-3834. https://doi.org/10.1007/s12274-023-6334-2
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Abstract Full text Electronic supplementary material About this article

Carbon-supported noble-metal-free single-atom catalysts (SACs) have aroused widespread interest due to their green chemistry aspects and excellent performances. Herein, we propose a “ligand regulation strategy” and achieve the successful fabrication of bifunctional SAC/MOF (MOF = metal–organic framework) nanocomposite (abbreviated NiSA/ZIF-300; ZIF = ZIF-8) with exceptional catalytic performance and robustness. The designed NiSA/ZIF-300 has a planar interfacial structure with the Ni atom, involving one S and three N atoms bonded to Ni(II), fabricated by controllable pyrolysis of volatile Ni-S fragments. For CO2 cycloaddition to styrene epoxide, NiSA/ZIF-300 exhibits ultrahigh activity (turnover number (TON) = 1.18 × 105; turnover frequency (TOF) = 9830 molSC·molNi−1·h−1; SC = styrene carbonate) and durability at 70 °C under 1 atm CO2 pressure, which is much superior to Ni complex/ZIF, NiNP/ZIF-300, and most reported catalysts. This study offers a simple method of bifunctional SAC/MOF nanocomposite fabrication and usage, and provides guidance for the precise design of additional original SACs with unique catalytic properties.


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Abstract
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Electronic supplementary material
About this article

Design of bifunctional single-atom catalysts NiSA/ZIF-300 for CO2 conversion by ligand regulation strategy

Show Author's information Wengang Fu1,§, Yapei Yun1,§, Hongting Sheng1( ), Xiaokang Liu3, Tao Ding3, Shuxian Hu4, Tao Yao3, Binghui Ge1, Yuanxin Du1, Didier Astruc2( ), Manzhou Zhu1,5( )
Department of Chemistry and Centre for Atomic Engineering of Advanced Materials, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, College of Materials Science and Engineering, Institutes of Physical Science and Information Technology and Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized Materials, Anhui University, Hefei 230601, China
Université de Bordeaux, ISM, UMR CNRS N°5255, 351 Cours de La Libération, 33405 Talence Cedex, France
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230026, China
Department of Physics, University of Science and Technology Beijing, Beijing 100083, China
Anhui Tongyuan Environment Energy Saving Co., Ltd, Hefei 230041, China

§ Wengang Fu and Yapei Yun contributed equally to this work.

Abstract

Carbon-supported noble-metal-free single-atom catalysts (SACs) have aroused widespread interest due to their green chemistry aspects and excellent performances. Herein, we propose a “ligand regulation strategy” and achieve the successful fabrication of bifunctional SAC/MOF (MOF = metal–organic framework) nanocomposite (abbreviated NiSA/ZIF-300; ZIF = ZIF-8) with exceptional catalytic performance and robustness. The designed NiSA/ZIF-300 has a planar interfacial structure with the Ni atom, involving one S and three N atoms bonded to Ni(II), fabricated by controllable pyrolysis of volatile Ni-S fragments. For CO2 cycloaddition to styrene epoxide, NiSA/ZIF-300 exhibits ultrahigh activity (turnover number (TON) = 1.18 × 105; turnover frequency (TOF) = 9830 molSC·molNi−1·h−1; SC = styrene carbonate) and durability at 70 °C under 1 atm CO2 pressure, which is much superior to Ni complex/ZIF, NiNP/ZIF-300, and most reported catalysts. This study offers a simple method of bifunctional SAC/MOF nanocomposite fabrication and usage, and provides guidance for the precise design of additional original SACs with unique catalytic properties.

Keywords: catalyst, CO2 conversion, cycloaddition, single atom, bifunctional

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Publication history
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Acknowledgements

Publication history

Received: 14 September 2023
Revised: 01 November 2023
Accepted: 13 November 2023
Published: 12 December 2023
Issue date: May 2024

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

We acknowledge the financial support by the National Natural Science Foundation of China (Nos. 21972001 and 21871001), the Natural Science Foundation of Anhui Province (No. 2008085MB37), the Anhui University, the University of Bordeaux, and the Centre National de la Recherche Scientifique (CNRS).

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