第一性原理计算研究 LiAl(OH)Cl 的电子结构和锂离子扩散。

Electronic Structure and Lithium Diffusion in LiAl(OH)Cl Studied by First Principle Calculations.

机构信息

State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter (FJIRSM) Chinese Academy of Sciences (CAS), Fuzhou 350002, China.

Max-Planck-Institute for Solid State Research, Heisenbergstr. 1, D-70569 Stuttgart, Germany.

出版信息

Molecules. 2019 Jul 23;24(14):2667. doi: 10.3390/molecules24142667.

DOI:10.3390/molecules24142667

PMID:31340539

原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC6681411/

Abstract

First-principles calculations based on the density functional theory (DFT) were carried out to study the atomic structure and electronic structure of LiAl(OH)Cl, the only material in the layered double hydroxide family in which delithiation was found to occur. Ab initio molecular dynamics (AIMD) simulations were used to explore the evolution of the structure of LiAl(OH)Cl during a thermally induced delithiation process. The simulations show that this process occurs due to the drastic dynamics of Li at temperatures higher than ~450 K, in which the [Al(OH)] host layers remain stable up to 1100 K. The calculated large value of the Li diffusion coefficient D, ~ 3.13 × 10 - 5 c m 2 / s , at 500 K and the high stability of the [Al(OH)] framework suggest a potential technical application of the partially-delithiated LiAl(OH)Cl (0 < x < 1) as a superionic conductor at high temperatures.

摘要

基于密度泛函理论（DFT）的第一性原理计算研究了 LiAl(OH)Cl 的原子结构和电子结构，LiAl(OH)Cl 是层状双氢氧化物家族中唯一发现脱锂的材料。采用从头算分子动力学（AIMD）模拟研究了在热诱导脱锂过程中 LiAl(OH)Cl 结构的演变。模拟表明，在高于约 450 K 的温度下，由于 Li 的剧烈动力学，导致了这一过程的发生，在该温度下，[Al(OH)]主体层在高达 1100 K 的温度下保持稳定。在 500 K 时计算得到的 Li 扩散系数 D 的较大值，约为 3.13×10 - 5 c m 2 / s ，以及 [Al(OH)] 骨架的高稳定性表明，部分脱锂的 LiAl(OH)Cl（0 < x < 1）作为高温下的超离子导体具有潜在的技术应用前景。