Liquid organic hydrogen carriers (LOHC) are interesting hydrogen vectors which can exploit existing infrastructure. Specifically, N-heterocyclic compounds are attractive due to lower dehydrogenation enthalpy than homocyclic ones and demand a viable palladium catalyst to guarantee high dehydrogenation activity at low temperatures and stability in recycle runs. Here, we employ one-pot solvent deficient precipitation yielding a mesoporous palladium-alumina. The prepared catalyst system offers higher hydrogen release capability by 20% than conventional palladium/γ-Al₂O₃ in the dehydrogenation of four different N-heterocyclic compounds at or below 250 °C. Futhermore, it shows negligible activity loss up to five consecutive runs for perhydro 2-(n-methylbenzyl)pyridine and perhydro 2-methylindole. Such dehydrogenation performance is caused by the solvent deficient environment that restricts palladium mobility by contiguous alumina particles and produces well-dispersed palladium phase with a higher density of (111) plane. Therefore, the reported synthesis method may contribute to the production of innovative dehydrogenation catalysts for LOHC compounds.

Decalin is more easily dehydrogenated on Pt catalyst than Pd while the dehydrogenation of tetralin is more facile on Pd than Pt.