Polar O-Co-P Surface for Bimolecular Activation in Catalytic Hydrogen Generation

Boron hydrides release an abundant amount of hydrogen in the presence of a suitable catalyst.Accelerating bimolecular activation kinetics is the key to designing cost-effective catalysts for borohydride hydrolysis.In this study,the bimolecular activation of a polar O-Co-P site demonstrated superior hydrogen-generation kinetics(turnover frequency,TOF=37 min−1,298 K)and low activation energy(41.0 kJ mol^(−1))close to that of noble-metal-based catalysts.Through a combination of experiments and theoretical calculations,it was revealed that the activated dangling oxygen atom in the Co–O precursor effectively replaced via surface-phosphorization because of strong electronic interactions between the dangling oxygen and P atoms.This substitution modulated the local coordination environment and electronegativity around the surface Co sites and formed a new polar O-Co-P active site for optimizing the activation kinetics of ammonia borane and water.This strategy based on bimolecular activation may create new avenues in the field of catalysis.