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Hollow mesoporous atomically dispersed metal-nitrogen-carbon catalysts with enhanced diffusion for catalysis involving larger molecules

Author

Listed:
  • Xu Han

    (Beijing University of Chemical Technology)

  • Tianyu Zhang

    (Beijing University of Chemical Technology)

  • Xinhe Wang

    (Beijing University of Chemical Technology)

  • Zedong Zhang

    (Beijing University of Chemical Technology)

  • Yaping Li

    (Beijing University of Chemical Technology)

  • Yongji Qin

    (Beijing University of Chemical Technology)

  • Bingqing Wang

    (Beijing University of Chemical Technology)

  • Aijuan Han

    (Beijing University of Chemical Technology)

  • Junfeng Liu

    (Beijing University of Chemical Technology)

Abstract

Single-atom catalysts (SACs) show great promise in various applications due to their maximal atom utilization efficiency. However, the controlled synthesis of SACs with appropriate porous structures remains a challenge that must be overcome to address the diffusion issues in catalysis. Resolving these diffusion issues has become increasingly important because the intrinsic activity of the catalysts is dramatically improved by spatially isolated single-atom sites. Herein, we develop a facile topo-conversion strategy for fabricating hollow mesoporous metal-nitrogen-carbon SACs with enhanced diffusion for catalysis. Several hollow mesoporous metal-nitrogen-carbon SACs, including Co, Ni, Mn and Cu, are successfully fabricated by this strategy. Taking hollow mesoporous cobalt-nitrogen-carbon SACs as a proof-of-concept, diffusion and kinetic experiments demonstrate the enhanced diffusion of hollow mesoporous structures compared to the solid ones, which alleviates the bottleneck of poor mass transport in catalysis, especially involving larger molecules. Impressively, the combination of superior intrinsic activity from Co-N4 sites and the enhanced diffusion from the hollow mesoporous nanoarchitecture significantly improves the catalytic performance of the oxidative coupling of aniline and its derivatives.

Suggested Citation

  • Xu Han & Tianyu Zhang & Xinhe Wang & Zedong Zhang & Yaping Li & Yongji Qin & Bingqing Wang & Aijuan Han & Junfeng Liu, 2022. "Hollow mesoporous atomically dispersed metal-nitrogen-carbon catalysts with enhanced diffusion for catalysis involving larger molecules," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-30520-3
    DOI: 10.1038/s41467-022-30520-3
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    References listed on IDEAS

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    1. Xiaohui He & Qian He & Yuchen Deng & Mi Peng & Hongyu Chen & Ying Zhang & Siyu Yao & Mengtao Zhang & Dequan Xiao & Ding Ma & Binghui Ge & Hongbing Ji, 2019. "A versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
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    Cited by:

    1. Haidong Xu & Ji Han & Bin Zhao & Ruigang Sun & Guiyuan Zhong & Guangrui Chen & Yusuke Yamauchi & Buyuan Guan, 2023. "A facile dual-template-directed successive assembly approach to hollow multi-shell mesoporous metal–organic framework particles," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Jie Zhang & Linshan Liu & Chaofeng Zheng & Wang Li & Chunru Wang & Taishan Wang, 2023. "Embedded nano spin sensor for in situ probing of gas adsorption inside porous organic frameworks," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    3. Shujuan Liu & Teng Li & Feng Shi & Haiying Ma & Bin Wang & Xingchao Dai & Xinjiang Cui, 2023. "Constructing multiple active sites in iron oxide catalysts for improving carbonylation reactions," Nature Communications, Nature, vol. 14(1), pages 1-13, December.

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