He Zhe, Li Kailang, Chen Tianxiang, Feng Yunchao, Villalobos-Portillo Eduardo, Marini Carlo, Lo Tsz Woon Benedict, Yang Fuyuan, Zhang Liang, Liu Lichen
Engineering Research Center of Advanced Rare-Earth Materials of Ministry of Education, Department of Chemistry, Tsinghua University, Beijing, China.
Center for Combustion Energy, Tsinghua University, Beijing, China.
Nat Commun. 2025 Jan 2;16(1):92. doi: 10.1038/s41467-024-55370-z.
Liquid organic hydrogen carriers (LOHCs) are considered promising carriers for large-scale H 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 storage/transportation plants based on the toluene-methylcyclohexane cycle relies on the use of high-performance catalysts, especially for the H 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 with purity >99.9%), remarkably high stability (>2000 h) and regenerability over consecutive reaction-regeneration cycles.
液态有机氢载体（LOHCs）被认为是大规模储氢和输氢的有前景的载体，其中甲苯 - 甲基环己烷循环因其低成本以及与当前化学品运输基础设施的兼容性而受到工业界和学术界的高度关注。基于甲苯 - 甲基环己烷循环的储氢/输氢工厂的大规模部署依赖于高性能催化剂的使用，特别是用于通过甲基环己烷脱氢进行氢释放的过程。在这项工作中，我们通过在刚性沸石基质中引入具有精确控制的组成和位置的亚纳米PtFe团簇，开发了一种用于甲基环己烷脱氢反应的高效催化剂。所得的沸石封装的PtFe团簇在甲基环己烷脱氢生成甲苯的反应中表现出目前最高的反应速率、对甲苯非常高的化学选择性（能够生产纯度>99.9%的氢气）、显著高的稳定性（>2000小时）以及在连续反应 - 再生循环中的可再生性。
