Novel activated carbon supported trimetallic PdCoAg nanoparticles as efficient catalysts for the hydrolytic dehydrogenation of ammonia borane

被引:44
作者
Kazici, Hilal Celik [1 ]
Yildiz, Fikret [1 ]
Izgi, Mehmet Sait [2 ]
Ulas, Berdan [1 ]
Kivrak, Hilal [1 ]
机构
[1] Van Yuzuncu Yil Univ, Dept Chem Engn, Fac Engn, TR-65080 Van, Turkey
[2] Siirt Univ, Dept Chem Engn, Fac Engn, TR-56100 Siirt, Turkey
关键词
Ammonia borane; Palladium cobalt silver nanoparticles; Activated carbon; Hydrolysis; Hydrogen; Heterogeneous catalysis; CORE-SHELL NANOPARTICLES; IN-SITU SYNTHESIS; HYDROGEN GENERATION; SODIUM-BOROHYDRIDE; GRAPHENE OXIDE; PERSPECTIVE; PERFORMANCE; PROGRESS; ALLOYS; CERIA;
D O I
10.1016/j.ijhydene.2019.02.198
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
Activated carbon (AC) supported palladium, cobalt and silver nanoparticle (PdCoAg/AC) catalysts were prepared by in situ reduction of sodium borohydride (NaBH4) and characterized by various techniques such as X-ray diffraction (XRD), scanning electron microscope (SEM) and energy-dispersive X-ray spectroscopy (EDX), Transmission electron microscopy (TEM) and X-ray Photoelectron Spectroscopy (XPS). The PdCoAg/AC catalyst is active in the hydrolysis of ammonia-borane (AB) even at low temperatures. Compared with mono- (Pd) and bi-metallic (PdCo) nanoparticles, this trimetallic (PdCoAg) structure showed greatly increased catalytic activity for AB hydrolysis. Their hydrolysis completion time was 50 s. This study also included full experimental details of kinetic data to determine the activation parameters (Ea, Delta H and Delta S) for the rate law and the catalytic hydrolysis of AB. In addition, the PdCoAg/AC catalysts had favorable catalytic activity also after seven runs. Hydrogen generation rate (HG), Ea, Delta H and Delta S were obtained at 25 degrees C as 4666.66 mL min(-1)g(-1) (2 mmol AB and 50 mg PdCoAg/AC), 26.836 kJ mol(-1), 29.416 kJ mol(-1) and -108.42 J mol(-1)K(-1), respectively. In addition, the study showed that Pd0.6Co0.2CAg0.2/AC (Pd:Co:Ag atomic ratio = 6:2:2) showed the total turnover frequency (TOF) value of 6624 h(-1). These results demonstrate that the PdCoAg/AC catalyst is a promising alternative in search of the practical application of AB as a hydrogen storage material for fuel cell applications. (C) 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
引用
收藏
页码:10561 / 10572
页数:12
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