Premium
A New Lithium‐Ion Conductor LiTaSiO 5 : Theoretical Prediction, Materials Synthesis, and Ionic Conductivity
Author(s) -
Wang Qi,
Wu JianFang,
Lu Ziheng,
Ciucci Francesco,
Pang Wei Kong,
Guo Xin
Publication year - 2019
Publication title -
advanced functional materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 6.069
H-Index - 322
eISSN - 1616-3028
pISSN - 1616-301X
DOI - 10.1002/adfm.201904232
Subject(s) - materials science , lithium (medication) , ion , electrolyte , ionic conductivity , neutron diffraction , chemical physics , conductivity , doping , ionic bonding , fast ion conductor , ab initio , inorganic chemistry , chemistry , crystallography , crystal structure , electrode , organic chemistry , optoelectronics , endocrinology , medicine
Owing to the nonleakage and incombustibility, solid electrolytes are crucial for solving the safety issues of rechargeable lithium batteries. In this work, a new class of solid electrolyte, acceptor‐doped LiTaSiO 5 , is designed and synthesized based on the concerted migration mechanism. When Zr 4+ is doped to the Ta 5+ sites in LiTaSiO 5 , the high‐energy lattice sites are partly occupied by the introduced lithium ions, and the lithium ions at those sites interact with the lithium ions placed in the low‐energy sites, thereby favoring the concerted motion of lithium ions and lowering the energy barrier for ion transport. Therefore, the concerted migration of lithium ions occurs in Zr‐doped LiTaSiO 5 , and a 3D lithium‐ion diffusion network is established with quasi‐1D chains connected through interchain channels. The lithium‐ion occupation, as revealed by ab initio calculations, is validated by neutron powder diffraction. Zr‐doped LiTaSiO 5 electrolytes are successfully synthesized; Li 1.1 Ta 0.9 Zr 0.1 SiO 5 shows a conductivity of 2.97 × 10 −5 S cm −1 at 25 °C, about two orders of magnitude higher than that of LiTaSiO 5 , and it increases to 3.11 × 10 −4 S cm −1 at 100 °C. This work demonstrates the power of theory in designing new materials.