Refined alteration of active sites via O modification on CoP/Co2P@Carbon hetero-structural catalyst for hydrogen generation

Elucidating the relationship between heterostructure and catalytic activity is scientifically significant for water-related dissociation reactions. Herein, oxygen (O) modified CoP/Co2P@carbon heterostructure (O-(CoP/Co2P)@SC) is deliberately designed through controlled O modification and Local P-inducing Strategy. The optimal catalyst presents potent catalytic activity (turnover frequency of 35 min−1) and the stability without abominable decrease even after long-time usage. The prominent catalytic activity stems from the successful construction and refined alteration of active sites (Co atoms in form of Co-P and Co-O). Combining experimental results and density functional theory simulations, the activation energies and reaction dissociation energies of reactants (NH3BH3 and H2O) are altered, thus to optimize the catalytic kinetics of NH3BH3 hydrolysis (active Co nearby Co-O activates H2O and active Co nearby Co-P activates NH3BH3). This O modification strategy brings new inspiration for boosting catalytic activity of transition metal phosphides