This study presents a durable Pt-based catalyst for the dehydrogenation of perhydro-monobenzyltoluene (H12-MBT), a key reaction in Liquid Organic Hydrogen Carrier (LOHC) systems. By inducing the synergistic effects of phosphorus and sulfur, the catalyst design enables selective sulfur adsorption onto Pt surfaces while minimizing overall sulfur usage. Phosphate doping plays a multifaceted role: it preoccupies acidic sites on the Al₂O₃ support, thereby promoting uniform Pt dispersion and suppressing undesirable sulfur migration. Moreover, the phosphate species contribute to electronic modulation of the catalytic system by adjusting the overall charge balance, which stabilizes the active Pt sites and facilitates favorable sulfur adsorption. The resulting partially positively charged Pt species exhibit improved catalytic activity and coke resistance. Among the developed catalysts, SPt/0.9PA demonstrated outstanding long-term stability and sustained high hydrogen production efficiency for over 100 hours. This work offers a promising strategy for the rational design of efficient and robust catalysts tailored for commercial LOHC-based hydrogen storage and release systems.
