Facile fabrication of poly(amidoamine) (PAMAM) dendrimers-encapsulated Ag-Co bimetallic nanoparticles for highly efficient dehydrogenation of ammonia borane

被引:43
作者
Ke, Dandan [1 ,2 ]
Li, Yuan [1 ,2 ]
Wang, Jin [1 ,2 ]
Zhang, Lu [1 ,2 ]
Wang, Jidong [1 ,2 ]
Zhao, Xin [3 ]
Yang, Shuqin [1 ,2 ]
Han, Shumin [1 ,2 ]
机构
[1] Yanshan Univ, Sch Environm & Chem Engn, Hebei Key Lab Appl Chem, Qinhuangdao 066004, Peoples R China
[2] Yanshan Univ, State Key Lab Metastable Mat Sci & Technol, Qinhuangdao 066004, Peoples R China
[3] Baotou Res Inst Rare Earths, Baotou 014030, Peoples R China
基金
中国国家自然科学基金;
关键词
PAMAM dendrimers; Ag-Co bimetallic nanoparticles; Hydrolytic dehydrogenation; Ammonia borane; HYDROGEN GENERATION; HYDROLYTIC DEHYDROGENATION; SHELL NANOPARTICLES; CATALYTIC-ACTIVITY; GRAPHENE; NI; REUSABILITY; COMPOSITES; CRYOGEL; NABH4;
D O I
10.1016/j.ijhydene.2015.11.142
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
Multifunctional poly(amidoamine) (PAMAM) dendrimers-encapsulated Ag-Co bimetallic nanoparticles (Ag-Co/PAMAM NPs) have been prepared via a facile co-complexation chemical reduction method. By exploiting the well-defined dendritic spatial construction of PAMAM dendrimers as NPs support and capping ligand, the as-synthesized NPs show unconspicuous agglomeration and uniformly distribution with average diameter of 5 nm. The Ag-Co/PAMAM NPs show the composition-dependent catalytic activity in catalytic dehydrogenation of ammonia borane (AB), with NPs in 30 atom.% Ag exhibiting the superior activity and yielding an initial turnover frequency (TOF) as high as 15.84 mol(H2 center dot)min(-1)center dot mol(M)(-1). Combined with the electro-transfer interaction between Ag and Co, the effective control of the NPs dispersibility and the electro-donating ability of PAMAM dendrimers with amounts of amide and amine groups facilitate the catalytic performances of Ag-Co/PAMAM catalyst on the hydrolysis of AB. The work also includes the kinetic studies on zero-order with respect to substrate concentration and first-order reaction with respect to catalyst concentration, as well as temperature effect to determine the apparent activation energy of the reaction (Ea = 35.66 kJ mol(-1)). Furthermore, the reusability tests reveal Ag-Co/PAMAM NPs still show good catalytic activity and magnetically reusability in successive runs, which make these dendrimers-stabilized bimetallic nanoparticles promising heterogeneous catalysts in practical application. Copyright (C) 2015, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
引用
收藏
页码:2564 / 2574
页数:11
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