Surface-bonded water in h-BN for synergistically triggering catalytic activity to hydrogen generation from ammonia borane via coordination dissociation

Abstract

Developing catalysts with efficient activity to the reaction systems with water dissociation represents a significant and challenging mission in chemistry. Herein, CoP nanosheets supported on h-BN with surface-bonded water (CoP/h-BN OH ) is designed through a P-inducing strategy to stimulate the activity toward hydrogen generation. Hydroxyl functional groups (−OH) binds to B sites preferentially on h-BN surface during the process of surface hydroxylation to form B OH . The P-inducing strategy modulates the electronic configuration nearby Co and combines with B OH to facilitate the catalytic activity. The optimal catalyst exhibits a state-of-the-art turnover frequency (TOF) of 43 min −1 with considerable stability in NH 3 BH 3 hydrolysis. The rapid hydrogen generation during NH 3 BH 3 hydrolysis is ascribed to the integration of the active sites of B OH and CoP. Both experiments and theory demonstrate that reactant molecules (NH 3 BH 3 and H 2 O) adsorption and dissociation are mediated by the existence of B OH and CoP dual-active sites (B OH activates H 2 O, Co-P activates NH 3 BH 3 ). This work sheds fresh light on the design of efficient non-noble catalysts and motivates the exploration of hydrogen energy utilization technologies. CoP nanosheet supported on h-BN with surface-bonded water (CoP/h-BN OH ) is designed through a P-inducing strategy to stimulate the catalytic activity toward hydrogen generation. The catalyst exhibits a superior kinetics with favorable stability in hydrogen generation from ammonia borane hydrolysis. • CoP supported on h-BN with surface-bonded water was designed via a P-inducing strategy. • A TOF of 43 min −1 was achieved for NH 3 BH 3 hydrolysis on dual-active sites. • DFT calculation revealed the catalytic mechanism of B OH and CoP in hydrolysis reaction.