Monodisperse nickel-palladium alloy nanoparticles supported on reduced graphene oxide as highly efficient catalysts for the hydrolytic dehydrogenation of ammonia borane

被引:59
作者
Ciftci, Nesibe Sedanur [1 ]
Metin, Onder [1 ]
机构
[1] Ataturk Univ, Fac Sci, Dept Chem, TR-25240 Erzurum, Turkey
关键词
Nickel; Palladium; Alloy nanoparticles; Reduced graphene oxide; Ammonia borane; Dehydrogenation; CHEMICAL HYDROGEN STORAGE; REUSABLE CATALYST; FACILE SYNTHESIS; AMINE-BORANE; NANOCLUSTERS; GENERATION;
D O I
10.1016/j.ijhydene.2014.09.060
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Addressed herein is the catalysis of reduced graphene oxide-supported monodisperse NiPd alloy nanoparticles (NPs) (rGO-NiPd) in the hydrolytic dehydrogenation of ammonia borane (AB). This is the first example of the use of NiPd alloy NPs as catalyst in the hydrolytic dehydrogenation of AB. Monodisperse NiPd alloy NPs (3.5 nm) were synthesized by co-reduction of nickel(II) acetate and palladium(II) acetylacetonate in oleylamine (OAm) and borane-tert-butylamine complex (BTB) at 100 degrees C. The current recipe allowed to control the composition of NiPd alloy NPs and to study the composition-controlled catalysis of rGO-NiPd in the hydrolytic dehydrogenation of AB. Among the all compositions tested, the Ni30Pd70 was the most active one with the turnover frequency of 28.7 min(-1). The rGO-Ni30Pd70 were also durable catalysts in the hydrolytic dehydrogenation of AB providing 3650 total turnovers in 35 h and reused at six times without deactivation. The detailed reaction kinetics of hydrolytic dehydrogenation of AB revealed that the reaction proceeds first order with respect to the NiPd concentration and zeroth order with respect to the AB concentration. The apparent activation energy of the catalytic dehydrogenation of AB was also calculated to be E-a(app)=45 +/- 2 kJ*mol(-1). Copyright (C) 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
引用
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页码:18863 / 18870
页数:8
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