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Remarkable catalysis of spinel ferrite XFe2O4(X=Ni,Co,Mn,Cu,Zn)nanoparticles on the dehydrogenation properties of LiAlH_(4):An experimental and theoretical study

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Journal of Materials Science & Technology 2022年第16期111卷 189-203页

作者： Sheng Wei Jiaxi Liu Yongpeng Xia Huanzhi Zhang Riguang Cheng Lixian Sun Fen Xu Pengru Huang Federico Rosei aleskey a.pimerzin Hans Jüergen Seifert Hongge Pan School of Material Science&Engineering Guangxi Key Laboratory of Information Materials and Guangxi Collaborative Innovation Center of Structure and Property for New Energy and MaterialsGuilin University of Electronic TechnologyGuilin 541004China School of Mechanical&Electrical Engineering Guilin University of Electronic TechnologyGuilin 541004China CentreÉnergie Matériaux et TélécommunicationsInstitut National de la Recherche Scientifique1650 Boul.Lionel BouletVarennesJ3×1S2QuébecCanada Samara State Technical University Samara443100Russia Institute for Applied Materials Karlsruhe Institute of TechnologyHermann von Helmholtz Platz 176344 Eggenstein LeopoldshafenGermany School of New Energy Science and Technology Xi’an Technological UniversityXi’an 710021China

Safe,compact,lightweight and cost-effective hydrogen storage is one of the main challenges that need to be addressed to effectively deploy the hydrogen economy.LiAlH_(4),as a solid-state hydrogen storage material,presents several advantages such as high hydrogen storage capacity,low price and abundant sources.Unfortunately,neither thermodynamic nor kinetic properties of dehydrogenation for LiAlH_(4)can fulfill the requirements of practical application.Thus,a series of spinel ferrite nanoparticles such as XFe_(2)O_(4)(X=Ni,Co,Mn,Cu,Zn,Fe)were prepared by using the modified thermal decomposition method,and then doped into LiAlH_(4)by using ball milling.Our results show that LiAlH_(4)doped with 7 wt%NiFe_(2)O_(4)starts to release hydrogen at 69.1°C,and the total amount of hydrogen released is 7.29 wt%before 300°C.The activation energies of the two-step hydrogen release reactions of LiAlH_(4)doped with 7 wt%NiFe_(2)O_(4)are 42.32 kJ mol^(-1)and 71.42 k J mol,which are 59.0%and 63.6%lower than those of as-received LiAlH_(4),respectively.Combining the density functional theory(DFT)calculations,we reveal that both the presence of Ni FeOand in-situ formed AlNiin ball-milling decrease the desorption energy barrier of Al-H bonding in LiAlH_(4)and accelerate the breakdown of Al-H bonding through the interfacial charge transfer and the dehybridization of the Al-H cluster.Thus,the experimental and theoretical results open a new avenue toward designing high effective catalysts applied to LiAlH_(4)as a candidate for hydrogen storage.

关键词： Hydrogen storage Lithium aluminum Spinel ferrite nanoparticles

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