Dehydrogenation Mechanism of Liquid Organic Hydrogen Carrier Materials: A Density Functional Theory Study

Storing hydrogen via liquid organic hydrogen carrier (LOHC) is one of well-known methods for chemical energy storage because it exhibits good performance in hydrogen storage by reversible reactions of hydrogenation and dehydrogenation. However, the mechanism of hydrogenation or dehydrogenation reaction in LOHC materials is still poorly understood. In this study, we analyzed the mechanism of dehydrogenation of a target material using density functional theory (DFT) calculations.

Benzyl toluene was selected as a representative material of the storage. We obtained a thermodynamic database of 196 intermediates and investigated plausible dehydrogenation pathways based on the information. The effect of doping N into benzyl toluene on the dehydrogenation mechanism was also assessed. Our findings will provide valuable insight for experimentalists to develop high-performance LOHC materials.