Engineering Bimodal Oxygen Vacancies and Pt to Boost the Activity Toward Water Dissociation

Abstract Water dissociation is the rate‐limiting step of several energy‐related reactions due to the high energy barrier required for breaking the oxygen–hydrogen bond. In this work, a bimodal oxygen vacancy (V O ) catalysis strategy is adopted to boost the efficient water dissociation on Pt nanoparticles. The single facet‐exposed TiO 2 surface and NiO x nanocluster possess two modes of V O different from each other. In ammonia borane hydrolysis, the highest catalytic activity among Pt‐based materials is achieved with the turnover frequency of 618 min −1 under alkaline‐free conditions at 298 K. Theoretical simulation and characterization analyses reveal that the bimodal V O significantly promotes the water dissociation in two ways. First, an ensemble‐inducing effect of Pt and V O in TiO 2 drives the activation of water molecules. Second, an electron promoter effect induced by the electron transfer from V O in NiO x to Pt further enhances the ability of Pt to dissociate water and ammonia borane. This insight into bimodal V O catalysis establishes a new avenue to rationally design heterogeneous catalytic materials in the energy chemistry field.