Cerium Oxide-Supported Positively Charged Platinum Single Atoms Enable Efficient Decalin Dehydrogenation under Mild Conditions

Abstract

Efficient decalin dehydrogenation is essential for hydrogen (H2) release in liquid organic hydrogen carrier (LOHC) systems.However, its strongly endothermic nature necessitates high temperatures, which promote aggregation of platinum (Pt) nanoparticles in conventional catalysts, leading to performance loss and high metal loading requirements. Addressing this challenge, we design a ceria-supported Pt single-atom catalyst (Pt SAC/CeO2) that maximizes atomic utilization and resists sintering through robust metal-support interactions and abundant oxygen vacancies. Integrated spectroscopic analyses and density functional theory (DFT) calculations reveal that these interactions generate positively charged Pt species that lower the activation barrier for the initial C-H bond scission and facilitate desorption of dehydrogenated aromatics, collectively enhancing catalytic efficiency. The optimized Pt SAC/CeO2 catalyst achieves an exceptional H2 production rate of 3126 mmol gPt -1 h -1 at 260 °C in a continuous-flow reactor, surpassing commercial Pt/C catalysts. Furthermore, coupling Pt SAC/CeO2 with a solar-thermal device enables sunlight-driven decalin dehydrogenation, delivering 3140 mmol gPt -1 h -1 under 0.5 kW m -2 and generating 11.6 L H2 per day without external power. Our study sheds light on charge modulation strategies for single-atom catalysts and provides a feasible pathway towards practical LOHC dehydrogenation processes.