Modulated noble metal/2D MOF heterostructures for improved hydrogen storage of MgH2

Zeng-Yi Li ¹Li-Xian Sun ¹Fen Xu ¹Yu-Mei Luo ¹Yong-Peng Xia ¹Sheng Wei ¹Chen-Chen Zhang ¹Ri-Guang Cheng ¹Chao-Feng Ye ¹Meng-Yuan Liu ¹Ju-Lan Zeng ²Zhong Cao ²Hong-Ge Pan³

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作者信息

1. School of Material Science and Engineering,Guilin University of Electronic Technology,Guilin 541004,China
2. School of Chemistry and Chemical Engineering,Changsha University of Science and Technology,Changsha 410114,China
3. Institute of Science and Technology for New Energy,Xi'an Technological University,Xi'an 710021,China
折叠

Abstract

The conjugation of external species with two-dimensional(2D)materials has broad application pro-spects.In this study,we have explored the potential of noble metal/2D MOF heterostructures in hydrogen storage.Specifically,the MgH2-Ni-MOF@Pd system has shown remarkable hydrogen desorption/sorption performances,starting to liberate hydrogen at 181 ℃,which is 230 ℃ lower than that of pristine MgH2.Under the catalytic effect of Ni-MOF@Pd,the dehydrogenation apparent activation energy of MgH2 is noticeably decreased from(133.5±17.5)to(34.58±1.87)kJ·mol-1,and the hydrogenation apparent activation energy is reduced from(70.41+7.43)to(25.78±4.64)kJ·mol-1,which is lowered by 63.4％.The fully-dehydrogenated MgH2-Ni-MOF@Pd composite rapidly uptakes hydrogen,with 2.62 wt％at 100 ℃ and 6.06 wt％at 150 ℃ within 300 s,respectively.The mechanism analysis of MgH2 catalyzed by Ni-MOF@Pd has revealed that the transformation of Mg2Ni and Mg2NiH4 could act as a"hydrogen pump",providing numerous channels for fast diffusion and trans-port of hydrogen atoms.Moreover,in the dehydrogenation process,the element Pd reacts with MgH2 to form the Mg-Pd alloy phase,which makes MgH2 take precedence to decompose through the Mg-Pd alloy rather than self-de-composition,further reducing thermal stability and improving de/hydrogenation kinetics.The synergistic effect of Mg-Pd,Mg2Ni,and the special ultra-thin 2D sheet structure of the additive is the main reason for the good hydrogen storage property of MgH2-Ni-MOF@Pd.Our findings provide inspiration for designing efficient multi-functional additives with unique morphologies to optimize the hydrogen desorption/sorption behaviors of hydrogen storage materials.

Key words

Hydrogen storage/Magnesium hydride/2D metal-organic framework nanosheets/Ni/Pd/Synergistic catalysis

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基金项目

National Natural Science Foundation of China(U20A20237)

National Natural Science Foundation of China(51863005)

National Natural Science Foundation of China(52271205)

National Natural Science Foundation of China(51871065)

National Natural Science Foundation of China(52371218)

National Natural Science Foundation of China(51863005)

National Natural Science Foundation of China(52271205)

National Natural Science Foundation of China(51871065)

National Natural Science Foundation of China(52371218)

National Natural Science Foundation of China(51971068)

National Natural Science Foundation of China(52101245)

Scientific Research and Technology Development Program of Guangxi(AA19182014)

Scientific Research and Technology Development Program of Guangxi(AD17195073)

Scientific Research and Technology Development Program of Guangxi(AA17202030-1)

Scientific Research and Technology Development Program of Guangxi(AB21220027)

Scientific Research and Technology Development Program of Guangxi(2021AB17045)

National Natural Science Foundation of Guangxi Province(2018GXNSFDA281051)

National Natural Science Foundation of Guangxi Province(2014GXNSFAA118401)

National Natural Science Foundation of Guangxi Province(2013GXNSFBA019244)

National Natural Science Foundation of Guangxi Province(2021GXNSFBA075057)

National Natural Science Foundation of Guangxi Province(2022GXNSFB A035632)

Scientific Research and Technology Development Program of Guilin(20210102-4)

Scientific Research and Technology Development Program of Guilin(20210216-1)

Guangxi Bagui Scholar Foundation,Guilin Lijiang Scholar Foundation()

Guangxi Collaborative Innovation Centre of Structure and Property for New Energy and Materials()

Guangxi Advanced Functional Materials Foundation()

Application Talents Small Highlands and Chinesisch-Deutsche Kooperationsgruppe(GZ1528)

出版年

2024

稀有金属(英文版)

中国有色金属学会

稀有金属(英文版)

CSTPCDCSCDEI

影响因子：0.801

ISSN：1001-0521

参考文献量65

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