Addressing the quantitative conversion bottleneck in single-atom catalysis

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.

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.