Electronic Structure and Lithium Diffusion in LiAl<sub>2</sub>(OH)<sub>6</sub>Cl Studied by First Principle Calculations
Yueping Zhang,
Xiyue Cheng,
Chen Wu,
Jürgen Köhler,
Shuiquan Deng
Affiliations
Yueping Zhang
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter (FJIRSM) Chinese Academy of Sciences (CAS), Fuzhou 350002, China
Xiyue Cheng
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter (FJIRSM) Chinese Academy of Sciences (CAS), Fuzhou 350002, China
Chen Wu
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter (FJIRSM) Chinese Academy of Sciences (CAS), Fuzhou 350002, China
Jürgen Köhler
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter (FJIRSM) Chinese Academy of Sciences (CAS), Fuzhou 350002, China
Shuiquan Deng
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter (FJIRSM) Chinese Academy of Sciences (CAS), Fuzhou 350002, China
First-principles calculations based on the density functional theory (DFT) were carried out to study the atomic structure and electronic structure of LiAl2(OH)6Cl, 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 LiAl2(OH)6Cl 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 [Al2(OH)6] 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 [Al2(OH)6] framework suggest a potential technical application of the partially-delithiated Li1-xAl2(OH)6Cl1-x (0 < x < 1) as a superionic conductor at high temperatures.
