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Research Article

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

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
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Graphical Abstract

Three kinds of morphologies (nanoparticles, nanocubes, and nanorods) of rare earth oxide nano-ceria are synthesized, characterized, and separately added to LiAlH4 to improve the dehydrogenation behavior. The influence of the nano-CeO2 intrinsic properties is clarified, and the dehydrogenation mechanism 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+.

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

hydrogen storageLiAlH4nano-CeO2morphology

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Nano Research
Volume 16 Issue 7,
July 2023
Pages 9426-9434
DOI: 10.1007/s12274-023-5636-8
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
Topics:
Hydrogen storage

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Received: 02 February 2023
Revised: 27 February 2023
Accepted: 02 March 2023
Published: 20 April 2023
© Tsinghua University Press 2023
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