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Biomass-assisted approach for large-scale construction of multi-functional isolated single-atom site catalysts

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Abstract

In recent years, the isolated single-atom site (ISAS) catalysts have attracted much attention as they are cost-effective, can achieve 100% atom-utilization efficiency, and often display superior catalytic performance. Here, we developed a biomass-assisted pyrolysis-etching-activation (PEA) strategy to construct ISAS metal decorated on N and B co-doped porous carbon (ISAS M/NBPC, M = Co, Fe, or Ni) catalysts. This PEA strategy can be applied in the universal and large-scale preparation of ISAS catalysts. Interestingly, the ISAS M/NBPC (M = Co, Fe, or Ni) catalysts show multi-functional features and excellent catalytic activities. They can be used to conduct different types of catalytic reactions, such as O-silylation (OSI), oxidative dehydrogenation (ODH), and transfer hydrogenation (THG). In addition, we used the transfer hydrogenation of nitrobenzene as a typical reaction and revealed the difference between ISAS Co/NBPC and ISAS Co/NPC (N-doped porous carbon) catalysts by density functional theory (DFT) calculations, and which showed that the decreased barrier of the ratedetermining step and the low-lying potential energy diagram indicate that the catalytic activity is higher when ISAS Co/NBPC is used than that when ISAS Co/NPC is used. These results demonstrate that the catalytic performance can be effectively improved by adjusting the coordination environment around the ISAS.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 21771003, 51902003, 21901007, 22002085, and 21501004), the University Synergy Innovation Program of Anhui Province (No. GXXT-2021-020), the Anhui Province Natural Science Foundation (Nos. 2008085QB53 and 2008085QB83), the Natural Science Research Project of Anhui Province Education Department (No. KJ2019A0581), the Open Project of Key Laboratory of Metallurgical Emission Reduction & Resources Recycling of Ministry of Education (No. JKF21-03), and the Open Foundation of Anhui Laboratory of Clean Catalytic Engineering (No. LCCE-01). We acknowledge the 1W1B beamline station of Beijing Synchrotron Radiation Facility (BSRF), and the Institute of Physics of Chinese Academy of Sciences. We acknowledge the National Synchrotron Radiation Laboratory (NSRL) of Hefei. We also thank Prof. Lirong Zheng, Prof. Wensheng Yan, Prof. Qinghua Zhang, and Prof. Jun Luo for their help in catalyst characterizations. Thanks to Prof. Chen Chen of Tsinghua University and Prof. Junjie Mao of Anhui Normal University for their help in materials characterizations and catalytic testing. We thank LetPub (www.letpub.com) for its linguistic assistance during the preparation of this manuscript.

Author information

Author notes

  1. Tao Wu, Sha Li, and Shoujie Liu contributed equally to this work.

Authors and Affiliations

  1. Key Laboratory of Metallurgical Emission Reduction & Resources Recycling, Ministry of Education, Institute of Clean Energy and Advanced Nanocatalysis (iClean), School of Chemistry and Chemical Engineering, Anhui University of Technology, Maanshan, 243002, China

    Tao Wu, Cheng Peng, Kai Yao, Yingping Li, Jieyue Wang, Xianwen Wei & Konglin Wu

  2. Anhui Laboratory of Clean Catalytic Engineering, School of Chemical and Environmental Engineering, Anhui Polytechnic University, Wuhu, 241000, China

    Tao Wu, Zhiming Chen & Konglin Wu

  3. Center of Single-Atom, Clusters, and Nanomaterials (CAN), College of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, China

    Tao Wu & Zheng Chen

  4. Chemistry and Chemical Engineering of Guangdong Laboratory, Shantou, 515063, China

    Sha Li & Shoujie Liu

  5. Department of Physics and Chemistry, Faculty of Science and Technology, University of Macau, Macao, China

    Weng-Chon Cheong

  6. School of Chemistry and Chemical Engineering, Anhui Key Laboratory of Photoelectric-Magnetic Functional Materials, Anqing Normal University, Anqing, 246011, China

    Binbin Jiang

Authors
  1. Tao Wu
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  2. Sha Li
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  3. Shoujie Liu
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  4. Weng-Chon Cheong
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  5. Cheng Peng
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  6. Kai Yao
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  7. Yingping Li
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  8. Jieyue Wang
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  9. Binbin Jiang
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  10. Zheng Chen
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  11. Zhiming Chen
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  12. Xianwen Wei
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  13. Konglin Wu
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Corresponding authors

Correspondence to Binbin Jiang, Zheng Chen or Konglin Wu.

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Wu, T., Li, S., Liu, S. et al. Biomass-assisted approach for large-scale construction of multi-functional isolated single-atom site catalysts. Nano Res. 15, 3980–3990 (2022). https://doi.org/10.1007/s12274-022-4091-2

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  • DOI: https://doi.org/10.1007/s12274-022-4091-2

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