Synergistic Pt-WO3 Dual Active Sites to Boost Hydrogen Production from Ammonia Borane

被引:47
|
作者
Chen, Wenyao [1 ]
Fu, Wenzhao [1 ]
Qian, Gang [1 ]
Zhang, Bingsen [2 ]
Chen, De [3 ]
Duan, Xuezhi [1 ]
Zhou, Xinggui [1 ]
机构
[1] East China Univ Sci & Technol, State Key Lab Chem Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China
[2] Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, 72 Wenhua Rd, Shenyang 110016, Peoples R China
[3] Norwegian Univ Sci & Technol, Dept Chem Engn, N-7491 Trondheim, Norway
基金
中国博士后科学基金;
关键词
CATALYZED HYDROLYTIC DEHYDROGENATION; INITIO MOLECULAR-DYNAMICS; TOTAL-ENERGY CALCULATIONS; CARBON NANOTUBES; PLATINUM NANOPARTICLES; KINETIC INSIGHTS; HIGHLY EFFICIENT; GRAPHENE OXIDE; GENERATION; EVOLUTION;
D O I
10.1016/j.isci.2020.100922
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
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.
引用
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页数:28
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