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

ABSTRACT Hydrogen (H 2 ) storage/release using dibenzyltoluene/perhydro‐dibenzyltoluene (DBT/H18‐DBT) provides a safe route for H 2 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 (CN Pt–O ). The Pt single atom catalyst (SAC) with CN Pt–O ≈ 4 on the step site of CeO 2 results in a unique reaction mechanism of preferential dehydrogenation of the H18‐DBT middle ring, enabling H 2 production from H18‐DBT at 200°C — a temperature far below those reported in the literature (≥ 260°C), which achieves a 7 times higher H 2 evolution rate () of 83430.0 mol H2 mol Pt −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.