Single Atom Catalysis Enables Preferential Middle-Ring Dehydrogenation of Perhydro-Dibenzyltoluene for Low-Temperature Hydrogen Production.

Hydrogen (H2) storage/release using dibenzyltoluene/perhydro-dibenzyltoluene (DBT/H18-DBT) provides a safe route for H2 transportation but suffers from high dehydrogenation temperature due to the large C-H dissociation energy of the H18-DBT side rings. In this work, we design a single Pt atom catalyst with well controlled Pt-O coordination number (CNPt-O). The Pt single atom catalyst (SAC) with CNPt-O ≈ 4 on the step site of CeO2 results in a unique reaction mechanism of preferential dehydrogenation of the H18-DBT middle ring, enabling H2 production from H18-DBT at 200°C - a temperature far below those reported in the literature (≥ 260°C), which achieves a 7 times higher H2 evolution rate ( r H 2 ) of 83430.0 molH2 molPt -1 h-1 at 300°C as compared to the published values with stable H18-DBT conversion of ∼90% during 50 repeated hydrogen storage/release cycles.