Electronic Structure and Lithium Diffusion in LiAl(2)(OH)(6)Cl Studied by First Principle Calculations

First-principles calculations based on the density functional theory (DFT) were carried out to study the atomic structure and electronic structure of LiAl(2)(OH)(6)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(2)(OH)(6)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(2)(OH)(6)] host layers remain stable up to 1100 K. The calculated large value of the Li(+) diffusion coefficient D, [Formula: see text] , at 500 K and the high stability of the [Al(2)(OH)(6)] framework suggest a potential technical application of the partially-delithiated Li(1-x)Al(2)(OH)(6)Cl(1-x) (0 < x < 1) as a superionic conductor at high temperatures.