4.8 Article

Addressing the quantitative conversion bottleneck in single-atom catalysis

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NATURE COMMUNICATIONS
卷 13, 期 1, 页码 -

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NATURE PORTFOLIO
DOI: 10.1038/s41467-022-30551-w

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  1. NRF-CRP grant Two-dimensional covalent organic framework [NRF-CRP16-2015-02]
  2. National Research Foundation, Prime Minister's Office, Singapore

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In this study, a flow chemistry approach was used to overcome the productivity bottleneck of single atom catalysts (SACs) in liquid-phase heterogeneous catalysis. The integration of Pt1-MoS2 SAC in a bench-top flow reactor resulted in a record productivity of multifunctional anilines, highlighting the potential of flow chemistry in increasing conversion rates and productivity of SACs.
The practical application of single atom catalyst (SAC) in liquid-phase heterogeneous catalysis is hampered by the productivity bottleneck as well as catalyst leaching. Here, a bench-top, fast-flow reactor integrated with Pt1-MoS2 SAC was fabricated for continuous production of multifunctional anilines (28 examples) at a record productivity of 5.8 g h-1. 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 cm(3)), with a Pt-1-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.

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