Cobalt Phosphide‐Supported Single‐Atom Pt Catalysts for Efficient and Stable Hydrogen Generation from Ammonia Borane Hydrolysis

Abstract Ammonia borane (AB) has emerged as a promising chemical hydrogen storage material. The development of efficient, stable, and cost‐effective catalysts for AB hydrolysis is the key to achieving hydrogen energy economy. Here, cobalt phosphide (CoP) is used to anchor single‐atom Pt species, acting as robust catalysts for hydrogen generation from AB hydrolysis. Thanks to the high Pt utilization and the synergy between CoP and Pt species, the optimized Pt/CoP‐100 catalyst exhibits an unprecedented hydrogen generation rate, giving a record turnover frequency (TOF) value of 39911 and turnover number of 2926829 at room temperature. These metrics surpass those of all existing state‐of‐the‐art supported metal catalysts by an order of magnitude. Density functional theory calculations reveal that the integration of single‐atom Pt onto the CoP substrate significantly enhances adsorption and dissociation processes for both water and AB molecules, thereby facilitating hydrogen production from AB hydrolysis. Interestingly, the TOF value is further elevated to 54878 under UV–vis light irradiation, which can be attributed to the efficient separation and mobility of photogenerated carriers at the Pt‐CoP interface. The findings underscore the effectiveness of CoP as a support for single‐atom metals in hydrogen production, offering insights for designing high‐performance catalysts for chemical hydrogen storage.