摘要：SummaryDevelopment of synergistic heterogeneous catalysts with active sites working cooperatively has been a pursuit of chemists. Herein, we report for the first time the fabrication and manipulation of Pt-WO3dual-active-sites to boost hydrogen generation from ammonia borane. A combination of DFT calculations, structural characterization, and kinetic (isotopic) analysis reveals that Pt and WO3act as the active sites for ammonia borane and H2O activation, respectively. A trade-off between the promoting effect of WO3and the negative effect of decreased Pt binding energy contributes to a volcano-shaped activity, and Pt/CNT-5W delivers a 4-fold increased activity of 710.1 molH2·molPt−1·min−1. Moreover, WO3is suggested to simultaneously act as the sacrificial site that can divert B-containing by-products away from Pt sites against deactivation, yielding an increase from 24% to 68% of the initial activity after five cycles. The strategy demonstrated here could shed a new light on the design and manipulation of dual-active-site catalysts.Graphical AbstractDisplay OmittedHighlights•Mechanism-guided design of Pt-WO3dual active sites boosts H2generation•A trade-off between WO3loading and Pt B.E. yields a volcano-shaped activity•WO3acts as the sacrificial site to divert by-products against deactivation•Multifunctional Pt-MO/C catalysts achieve enhanced activity and durabilityInorganic Chemistry; Catalysis; Nanomaterials
