High-purity hydrogen production from dehydrogenation of methylcyclohexane catalyzed by zeolite-encapsulated subnanometer platinum-iron clusters.

He, Zhe; Li, Kailang; Chen, Tianxiang; Feng, Yunchao; Villalobos-Portillo, Eduardo; Marini, Carlo; Lo, Tsz Woon Benedict; Yang, Fuyuan et al. · Nat Commun · 2025

basic_science · Level V

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Abstract

Liquid organic hydrogen carriers (LOHCs) are considered promising carriers for large-scale H<sub>2</sub> storage and transportation, among which the toluene-methylcyclohexane cycle has attracted great attention from industry and academia because of the low cost and its compatibility with the current infrastructure facility for the transportation of chemicals. The large-scale deployment of the H<sub>2</sub> storage/transportation plants based on the toluene-methylcyclohexane cycle relies on the use of high-performance catalysts, especially for the H<sub>2</sub> release process through the dehydrogenation of methylcyclohexane. In this work, we have developed a highly efficient catalyst for MCH dehydrogenation reaction by incorporating subnanometer PtFe clusters with precisely controlled composition and location within a rigid zeolite matrix. The resultant zeolite-encapsulated PtFe clusters exhibit the up-to-date highest reaction rate for dehydrogenation of methylcyclohexane to toluene, very high chemoselectivity to toluene (enabling the production of H<sub>2</sub> with purity >99.9%), remarkably high stability (>2000 h) and regenerability over consecutive reaction-regeneration cycles.