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Addressing the quantitative conversion bottleneck in single-atom catalysis

Author

Listed:
  • Zhongxin Chen

    (National University of Singapore)

  • Jingting Song

    (National University of Singapore
    International Campus of Tianjin University)

  • Rongrong Zhang

    (National University of Singapore
    International Campus of Tianjin University)

  • Runlai Li

    (Sichuan University)

  • Qikun Hu

    (National University of Singapore)

  • Pingping Wei

    (International Campus of Tianjin University
    National University of Singapore)

  • Shibo Xi

    (Institute of Chemical and Engineering Sciences, Agency for Science, Technology and Research (A*STAR))

  • Xin Zhou

    (National University of Singapore)

  • Phuc T. T. Nguyen

    (National University of Singapore)

  • Hai M. Duong

    (National University of Singapore)

  • Poh Seng Lee

    (National University of Singapore)

  • Xiaoxu Zhao

    (Peking University)

  • Ming Joo Koh

    (National University of Singapore)

  • Ning Yan

    (National University of Singapore)

  • Kian Ping Loh

    (National University of Singapore
    International Campus of Tianjin University)

Abstract

Single-atom catalysts (SACs) offer many advantages, such as atom economy and high chemoselectivity; however, their practical application in liquid-phase heterogeneous catalysis is hampered by the productivity bottleneck as well as catalyst leaching. Flow chemistry is a well-established method to increase the conversion rate of catalytic processes, however, SAC-catalysed flow chemistry in packed-bed type flow reactor is disadvantaged by low turnover number and poor stability. In this study, we demonstrate the use of fuel cell-type flow stacks enabled exceptionally high quantitative conversion in single atom-catalyzed reactions, as exemplified by the use of Pt SAC-on-MoS2/graphite felt catalysts incorporated in flow cell. A turnover frequency of approximately 8000 h−1 that corresponds to an aniline productivity of 5.8 g h−1 is achieved with a bench-top flow module (nominal reservoir volume of 1 cm3), with a Pt1-MoS2 catalyst loading of 1.5 g (3.2 mg of Pt). X-ray absorption fine structure spectroscopy combined with density functional theory calculations provide insights into stability and reactivity of single atom Pt supported in a pyramidal fashion on MoS2. Our study highlights the quantitative conversion bottleneck in SAC-mediated fine chemicals production can be overcome using flow chemistry.

Suggested Citation

  • Zhongxin Chen & Jingting Song & Rongrong Zhang & Runlai Li & Qikun Hu & Pingping Wei & Shibo Xi & Xin Zhou & Phuc T. T. Nguyen & Hai M. Duong & Poh Seng Lee & Xiaoxu Zhao & Ming Joo Koh & Ning Yan & K, 2022. "Addressing the quantitative conversion bottleneck in single-atom catalysis," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-30551-w
    DOI: 10.1038/s41467-022-30551-w
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    References listed on IDEAS

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    1. Haisheng Wei & Xiaoyan Liu & Aiqin Wang & Leilei Zhang & Botao Qiao & Xiaofeng Yang & Yanqiang Huang & Shu Miao & Jingyue Liu & Tao Zhang, 2014. "FeOx-supported platinum single-atom and pseudo-single-atom catalysts for chemoselective hydrogenation of functionalized nitroarenes," Nature Communications, Nature, vol. 5(1), pages 1-8, December.
    2. Zhongxin Chen & Kai Leng & Xiaoxu Zhao & Souradip Malkhandi & Wei Tang & Bingbing Tian & Lei Dong & Lirong Zheng & Ming Lin & Boon Siang Yeo & Kian Ping Loh, 2017. "Interface confined hydrogen evolution reaction in zero valent metal nanoparticles-intercalated molybdenum disulfide," Nature Communications, Nature, vol. 8(1), pages 1-9, April.
    3. Tian-Nan Ye & Zewen Xiao & Jiang Li & Yutong Gong & Hitoshi Abe & Yasuhiro Niwa & Masato Sasase & Masaaki Kitano & Hideo Hosono, 2020. "Stable single platinum atoms trapped in sub-nanometer cavities in 12CaO·7Al2O3 for chemoselective hydrogenation of nitroarenes," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
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    Cited by:

    1. Zhangliu Tian & Yumin Da & Meng Wang & Xinyu Dou & Xinhang Cui & Jie Chen & Rui Jiang & Shibo Xi & Baihua Cui & Yani Luo & Haotian Yang & Yu Long & Yukun Xiao & Wei Chen, 2023. "Selective photoelectrochemical oxidation of glucose to glucaric acid by single atom Pt decorated defective TiO2," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

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