Lignin jet fuel can be consisted of multiple species of cyclohexanes, where the hydrogen gas can be released through catalytic dehydrogenation. Meanwhile, this process can be reversed through rehydrogenation. Thus, lignin jet fuel can act as sustainable liquid organic hydrogen carrier (LOHC). In this work, we focus on designing Pt-based atomic clusters or nanoparticles for the dehydrogenation of decalin, a model compound of lignin jet fuel. By experiments, we first demonstrated that pure Pt atomic clusters or nanoparticles (e.g., 0.01 wt%, 0.1 wt%, 0.5 wt%, and 1.0 wt%, Pt the support of graphene) can be effective for the dehydrogenation of decalin. We revealed the catalyst particle size effect on the activity of dehydrogenation, where the Pt atomic clusters showed the highest turnover frequency. Second, we performed computational search of optimal dehydrogenation catalysts by doping transition metals (e.g., Cu and Ni) into Pt, using the inverse molecular design (IMD) approach. The IMD method pointed out that the PtCuNi atomic clusters or nanoparticles can be good catalysts for the dehydrogenation of decalin, where the cost of Pt catalysts can be reduced by the doping of transition metals. We conducted experimental synthesis and testing, verifying that the PtCuNi catalysts can be effective for decalin dehydrogenation. Our work will inspire the rational design of heterogeneous catalysts for dehydrogenation, for developing new LOHC technology based on lignin jet fuel for hydrogen production and storage.
