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Research Article

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

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.

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Graphical Abstract

A ligand regulation strategy provides an efficient and stable single-atom Ni catalyst (NiSA/ZIF-300) with NiS(N)3 planar structure, which was successfully prepared upon pyrolysis at 300 °C of volatile Ni–S fragments. NiSA/ZIF-300 shows excellent catalytic performance and robustness for the cycloaddition reaction of styrene oxide and CO2, far superior to various catalysts under different Ni environments.

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

single atomcatalystbifunctionalCO2 conversioncycloaddition

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Nano Research
Volume 17 Issue 5,
May 2024
Pages 3827-3834
DOI: 10.1007/s12274-023-6334-2
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
Topics:
Nanocatalysts

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Received: 14 September 2023
Revised: 01 November 2023
Accepted: 13 November 2023
Published: 12 December 2023
© Tsinghua University Press 2023
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