Abstract
Development 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-WO(3) dual-active-sites to boost hydrogen generation from ammonia borane. A combination of DFT calculations, structural characterization, and kinetic (isotopic) analysis reveals that Pt and WO(3) act as the active sites for ammonia borane and H(2)O activation, respectively. A trade-off between the promoting effect of WO(3) and 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 mol(H2)·mol(Pt)(-1)·min(-1). Moreover, WO(3) is 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.