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Nano Research 2023, 16(7): 9426-9434 https://doi.org/10.1007/s12274-023-5636-8
Research Article | Issue | Published: 20 April 2023

Dehydrogenation behavior and mechanism of LiAlH4 adding nano-CeO2 with different morphologies

Show Author's Information Chunmin Zhang1,2,  Long Liang1,2,  Shaolei Zhao1,2,  Zhijian Wu1,2,  Shaohua Wang3,4,  Dongming Yin1,  Qingshuang Wang5,  Limin Wang1,2,  Chunli Wang1( ),  Yong Cheng1( )
State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China
School of Applied Chemistry and Engineering, University of Science and Technology of China (USTC), Hefei 230023, China
National Engineering Research Center of Nonferrous Metals Materials and Products for New Energy, GRINM Group Co., Ltd., Beijing 100088, China
GRIMAT Engineering Institute Co., Ltd., Beijing 101407, China
College of Life Science and Technology, Changchun University of Science and Technology, Changchun 130022, China
Keywords:
morphology, hydrogen storage, LiAlH4, nano-CeO2
Topics:
Hydrogen storage
Cite this article:
Zhang C, Liang L, Zhao S, et al. Dehydrogenation behavior and mechanism of LiAlH4 adding nano-CeO2 with different morphologies. Nano Research, 2023, 16(7): 9426-9434. https://doi.org/10.1007/s12274-023-5636-8
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Abstract Full text Electronic supplementary material About this article

Complex hydride LiAlH4, as a hydrogen storage material, possesses high theoretical hydrogen storage capacity (10.5 wt.%). However, highly efficient additives are urgently required to modify its thermal stability and sluggish kinetics. Some additives exhibit unique morphology-dependent characteristics. Herein, the efficient rare earth oxide nano-CeO2 additives with different morphologies (nanoparticles, nanocubes, and nanorods) are prepared by the hydrothermal method, and the intrinsic properties are characterized. The three different morphologies of nano-CeO2, which are different in the Ce3+ content and specific surface area, are added to LiAlH4 to improve the dehydrogenation behavior. The LiAlH4-CeO2-nanorod composite exhibits the optimal dehydrogenation behavior, which begins to desorb hydrogen at 76.6 °C with a hydrogen capacity of 7.17 wt.%, and 3.83 wt.% hydrogen is desorbed within 30 min at 140 °C. The dehydrogenation process of the composites demonstrates that hydrogen release is facilitated by the in-situ formed CeH2.73 and the facile transition between the oxidation states of Ce4+ and Ce3+. Combined with density functional theory calculations, the addition of nano-CeO2 can weaken the Al–H bond and accelerate the decomposition of [AlH4]4− tetrahedron, which is consistent with the reduction of the decomposition activation energy.


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About this article

Dehydrogenation behavior and mechanism of LiAlH4 adding nano-CeO2 with different morphologies

Show Author's information Chunmin Zhang1,2, Long Liang1,2, Shaolei Zhao1,2, Zhijian Wu1,2, Shaohua Wang3,4, Dongming Yin1, Qingshuang Wang5, Limin Wang1,2, Chunli Wang1( ), Yong Cheng1( )
State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China
School of Applied Chemistry and Engineering, University of Science and Technology of China (USTC), Hefei 230023, China
National Engineering Research Center of Nonferrous Metals Materials and Products for New Energy, GRINM Group Co., Ltd., Beijing 100088, China
GRIMAT Engineering Institute Co., Ltd., Beijing 101407, China
College of Life Science and Technology, Changchun University of Science and Technology, Changchun 130022, China

Abstract

Complex hydride LiAlH4, as a hydrogen storage material, possesses high theoretical hydrogen storage capacity (10.5 wt.%). However, highly efficient additives are urgently required to modify its thermal stability and sluggish kinetics. Some additives exhibit unique morphology-dependent characteristics. Herein, the efficient rare earth oxide nano-CeO2 additives with different morphologies (nanoparticles, nanocubes, and nanorods) are prepared by the hydrothermal method, and the intrinsic properties are characterized. The three different morphologies of nano-CeO2, which are different in the Ce3+ content and specific surface area, are added to LiAlH4 to improve the dehydrogenation behavior. The LiAlH4-CeO2-nanorod composite exhibits the optimal dehydrogenation behavior, which begins to desorb hydrogen at 76.6 °C with a hydrogen capacity of 7.17 wt.%, and 3.83 wt.% hydrogen is desorbed within 30 min at 140 °C. The dehydrogenation process of the composites demonstrates that hydrogen release is facilitated by the in-situ formed CeH2.73 and the facile transition between the oxidation states of Ce4+ and Ce3+. Combined with density functional theory calculations, the addition of nano-CeO2 can weaken the Al–H bond and accelerate the decomposition of [AlH4]4− tetrahedron, which is consistent with the reduction of the decomposition activation energy.

Keywords: morphology, hydrogen storage, LiAlH4, nano-CeO2

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Publication history
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Acknowledgements

Publication history

Received: 02 February 2023
Revised: 27 February 2023
Accepted: 02 March 2023
Published: 20 April 2023
Issue date: July 2023

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was supported by the National Key R&D Program of China (No. 2021YFB4000604), National Science and Technology Major Project (No. 2020YFE0204500), Youth Growth Science and Technology Program of Jilin Province (No. 20220508001RC), Major Science and Technology Project of Inner Mongolia (No. 2021ZD0029), Youth Innovation Promotion Association CAS (Nos. 2021225 and 2022225), and Independent Research Project of the State Key Laboratory of Rare Earth Resources Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences (No. 110000RL86).

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