Single-atom Pt in intermetallics as an ultrastable and selective catalyst for propane dehydrogenation

Abstract

Propylene production via propane dehydrogenation (PDH) requires high reaction temperatures to obtain sufficient propylene yields, which results to prominent catalyst deactivation due to coke formation. Developing highly stable catalysts for PDH without deactivation even at high temperatures is of great interest and benefit for industry. Here, we report that single-atom Pt included in thermally stable intermetallic PtGa works as an ultrastable and selective catalyst for PDH at high temperatures. Intermetallic PtGa displays three-hold-Pt ensembles and single Pt atoms isolated by catalytically inert Ga at the surface, the former of which can be selectively blocked and disabled by Pb deposition. The PtGa-Pb/SiO2 catalyst exhibits 30% conversion with 99.6% propylene selectivity at 600 °C for 96 h without lowering the performance. The single-atom Pt well catalyzes the first and second C–H activation, while effectively inhibits the third one, which minimizes the side reactions to coke and drastically improves the selectivity and stability.

Heterogeneous alkane dehydrogenation catalysts investigated via a surface organometallic chemistry approach

“…In future these well-defined model systems could be used to explore the possibility of further optimized ternary systems, similar to those described in the recent literature. 123 In summary, SOMC provides unprecedented insight into the molecular-level structure of heterogeneous catalysts for light alkane dehydrogenation, informing strategies for the synthesis of improved catalytic systems, and providing a basis for understanding of the subtle interplay between structure and reactivity. As spectroscopic, computational and data-driven highthroughput experimentation approaches improve, we envisage that the insights provided using this approach will serve as a platform for the systematic study of new materials for the dehydrogenation of light alkanes.…”

Single‐Atom Catalysts: A Sustainable Pathway for the Advanced Catalytic Applications

“…[339] Pt-SA dispersed on Cu nanoparticles enhanced desorption of surface-bound propylene selectivity (90%) and excellent thermal stability for 120 h at 520 °C. Recently, PtGa-Pb/SiO 2 catalyst was also investigated for dehydrogenation of propane with the 30% conversion with 99.6% selectivity at 600 °C for 96 h, [340] which is higher than the Pt/Cu-SAA catalyst. [339] Epoxides such as styrene oxide, glycidol, etc.…”

“…[362] Few examples were reported to explore SACs for industrial relevant high temperature (>300 °C) gas-phase applications. [336,339,340,363] The thermal stability of SACs can be enhanced by strong interaction through a strong covalent metal-support interaction. [46] The controllable high-temperature shockwave strategy, [364] atom trapping, [365] and entropy-driven [366] methods were utilized to stabilize SA.…”

Design and tailoring of advanced catalytic process for light alkanes upgrading

“…As a result, it demonstrated much higher propylene selectivity ($90%) and excellent stability (>120 hours) under atmospheric pressure at 520 C. 130 Furukawa and coworkers designed and prepared the single-atom Pt in intermetallics catalyst (PtGa-Pb/SiO 2 ) by selectively blocking threefold hollow Pt 3 ensembles while maintaining the single-atom-like isolated Pt 1 sites, achieving a high selectivity of 99.6% for propylene production. 131 Weckhuysen and coworkers explored the Sndoped CeO 2 supported Pt single atom catalysts for this reaction. 132 The formation of Pt-Sn clusters under reaction conditions were found to be very stable, even during extended reaction at 680 C, enabling the achievement of high selectivity toward propylene production.…”