期刊
ISCIENCE
卷 23, 期 3, 页码 -出版社
CELL PRESS
DOI: 10.1016/j.isci.2020.100922
关键词
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资金
- Natural Science Foundation of China [21922803, 21776077]
- Shanghai Natural Science Foundation [17ZR1407300, 17ZR140750]
- China Postdoctoral Science Foundation [BX20190116]
- Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning
- Shanghai Rising-Star Program [17QA1401200]
- State Key Laboratory of Organic-Inorganic Composites [oic-201801007]
- Open Project of State Key Laboratory of Chemical Engineering [SKLChe-15C03]
Development of synergistic heterogeneous catalystswith active sites working cooperatively has been a pursuit of chemists. Herein, we report for the first time the fabrication and manipulation of Pt-WO3 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 WO3 act as the active sites for ammonia borane and H2O activation, respectively. A trade-off between the promoting effect of WO3 and the negative effect of decreased Pt binding energy contributes to a volcano-shaped activity, and Pt/CNT-5Wdelivers a 4-fold increased activity of 710.1 mol(H2).mol(Pt)(-1).min(-1). Moreover, WO3 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.
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