Facile synthesis of Co/Pd supported by few-walled carbon nanotubes as an efficient bidirectional catalyst for improving the low temperature hydrogen storage properties of magnesium hydride

被引:101
|
作者
Liu, Meijia [1 ]
Xiao, Xuezhang [1 ,4 ]
Zhao, Shuchun [1 ]
Chen, Man [1 ]
Mao, Jianfeng [2 ]
Luo, Bosang [1 ]
Chen, Lixin [1 ,3 ]
机构
[1] Zhejiang Univ, Sch Mat Sci & Engn, State Key Lab Silicon Mat, Hangzhou 310027, Zhejiang, Peoples R China
[2] Univ Wollongong, Australian Inst Innovat Mat, Inst Superconducting & Elect Mat, Wollongong, NSW 2522, Australia
[3] Key Lab Adv Mat & Applicat Batteries Zhejiang Pro, Hangzhou 310013, Zhejiang, Peoples R China
[4] South China Univ Technol, Guangdong Prov Key Lab Adv Energy Storage Mat, Guangzhou 510640, Guangdong, Peoples R China
基金
中国国家自然科学基金;
关键词
TUBE-IN-TUBE; ENHANCED DEHYDROGENATION; DESORPTION PERFORMANCES; MG6PD ALLOY; MGH2; PD; KINETICS; NI; CO; DIFFUSION;
D O I
10.1039/c8ta12431k
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
Catalytic doping is important for enhancing the hydrogen storage performance of metal hydrides, but it is challenging to develop a single catalyst to enhance both hydrogen desorption and absorption to a certain degree. Herein, a bidirectional Co/Pd catalyst, homogeneously loaded on bamboo-shaped carbon nanotubes (Co/Pd@B-CNTs), showed superior catalytic effects, improving both the hydrogen desorption and absorption properties of MgH2 at relatively low temperatures. The MgH2-Co/Pd@B-CNTs composite starts to release hydrogen at 198.9 degrees C, which is 132.4 degrees C lower than as-milled MgH2. The hydrogen desorption activation energy for MgH2 is reduced from 178.00 to 76.66 kJ mol(-1) by the catalytic effects of Co/Pd@B-CNTs. The MgH2-Co/Pd@B-CNTs composite shows dramatically improved absorption kinetics; it rapidly uptakes 6.68 wt% H-2 within 10 s at 250 degrees C, and quickly absorbs 1.91 wt% H-2 within 100 s, even at a temperature as low as 50 degrees C. More importantly, a special mechanism for the bidirectional catalyst Co/Pd is proposed for the first time and discussed in detail. During the hydrogenation process, elemental Pd plays a dominant role in accelerating the preferential diffusion of hydrogen atoms at the Pd/Mg interface, while during dehydrogenation, phase transformation between Mg2Co and Mg2CoH5 as well as a Mg-Pd alloy becomes the crucial factor, facilitating the release of hydrogen atoms by decreasing the diffusion barrier. Moreover, novel structures of bamboo-shaped carbon nanotubes with a large diameter (>100 nm) and high specific surface area (146.8 m(2) g(-1)) allow the homogenous dispersion of Co/Pd NPs and enhance the direct contact with MgH2 particles.
引用
收藏
页码:5277 / 5287
页数:11
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