Atomistic mechanism of high ionic conductivity in lithium ytterbium-based halide solid electrolytes:A first-principles study

作     者：Limin Wang Wei Xiao Lu Sun Rong Yang Jinqiu Yu Ligen Wang Limin Wang;Wei Xiao;Lu Sun;Rong Yang;Jinqiu Yu;Ligen Wang

作者机构：State Key Laboratory of Nonferrous Metals and ProcessesChina GRINM Group Co.Ltd.Beijing100088China GRIMAT Engineering Institute Co.Ltd.Beijing101407China General Research Institute for Nonferrous MetalsBeijing100088China China Automotive Battery Research Institute Co.Ltd.Beijing101407China Rare Earth Functional Materials(Xiong'an)Innovation Center Co.Ltd.Xiong'an071700China 

出 版 物：《Journal of Rare Earths》 (稀土学报（英文版）)

年 卷 期：2024年第42卷第1期

页      面：155-162,I0006页

核心收录：

学科分类：0808[工学-电气工程] 081704[工学-应用化学] 08[工学] 0817[工学-化学工程与技术] 

基　　金：Project supported by the GRINM Innovation Fund Project(2020TS0301) Jilin Province Science and Technology Major Project(20210301021GX) National Natural Science Foundation of China(U21A2080) 

主　　题：Halide solid-state electrolytes Phase stability Ionic conductivity First-principles calculations Rare earths 

摘      要：As the next generation of commercial automotive power batteries begins replacing liquid lithium batteries,many look towards all-solid-state batteries to pioneer the ***-so lid-state batteries have attracted the attention of countless researchers around the world because of their high safety and high energy *** recent times,halide solid-state electrolytes have become a research hotspot within solid-state electrolytes because of their potentially superior *** this paper,in the framework of DFT,we investigated the atomic mechanisms of improving the ionic conductivity and stability of Li_(3)YbCl_(6).Our calculations show that both trigonal and orthorhombic Li_(3)YbCl_(6) exhibit wide electrochemical windows and metastable properties(100 meV/atomEhull0 meV/atom).However,the orthorhombic Li_(3)YbCl_(6) can be stabilized at high temperatures by taking the vibrational entropy into account,which is supported by the experimental ***,it is expected that because of the Yb/Li synergistic interactions that,due to their strong mutual coulomb repulsion,influence the Li^(+)transport behavior,the orthorhombic Li_(3)YbCl_(6) might have superior ionic conductivities with appropriate Li+migration paths determined by the Yb^(3+) ***,higher ionic conductivities can be obtained by regulating the random distribution of Li^(+) *** Li^(+)-deficiency can also largely increase the ionic conductivity by invoking *** study helps gain a deeper understanding of the laws that govern ionic conductivities and stabilities and provides a certain theoretical reference for the experimental development and design of halide solid-state electrolytes.