Strong Metal-Support Interaction makes Durable Catalysts

Liquid organic hydrogen carrier (LOHC) technology is a promising method for hydrogen storage and transportation by using a reversible hydrogenation–dehydrogenation cycle between aromatic compounds and naphthene, such as toluene and methylcyclohexane (MCH). A key issue in this technology is to improve the lifetime of the catalyst for MCH dehydrogenation. Here, we developed a TiO₂-supported Pt catalyst (Pt@TiO₂) by engineering a unique strong metal-support interaction (SMSI). For the first time, the monometallic Pt@TiO₂ catalyst delivers durable MCH dehydrogenation at 350 ^oC, without any deactivation observed within 500 h. MCH conversion of 94% and toluene selectivity of ~100% are achieved. Detailed electron microscopic and spectroscopic studies, supported by theoretical calculations, reveal that the excellent MCH dehydrogenation performance over Pt@TiO₂is attributed to in-situ generated TiO_x-Pt^δ+ interface induced by optimal SMSI, which immobilizes Pt nanoparticle (NP) onto TiO₂ surface and modulates electronic properties of Pt NP. MCH can be thus efficiently dehydrogenated and toluene is easily desorbed on the Pt NP surface. Our results expand the concept of classical SMSI and provide new insights into the rational design of durable supported metal catalysts based on unconventional SMSI.