TY - JOUR
T1 - A Series of Ternary Metal Chloride Superionic Conductors for High-Performance All-Solid-State Lithium Batteries
AU - Liang, Jianwen
AU - van der Maas, Eveline
AU - Luo, Jing
AU - Li, Xiaona
AU - Chen, Ning
AU - Adair, Keegan R.
AU - Li, Weihan
AU - Li, Junjie
AU - Hu, Yongfeng
AU - Liu, Jue
AU - Zhang, Li
AU - Zhao, Wenxuan
AU - Parnell, Steven
AU - Ganapathy, Swapna
AU - Wagemaker, Marnix
PY - 2022
Y1 - 2022
N2 - Understanding the relationship between structure, ionic conductivity, and synthesis is the key to the development of superionic conductors. Here, a series of Li3-3xM1+xCl6 (−0.14 < x ≤ 0.5, M = Tb, Dy, Ho, Y, Er, Tm) solid electrolytes with orthorhombic and trigonal structures are reported. The orthorhombic phase of Li–M–Cl shows an approximately one order of magnitude increase in ionic conductivities when compared to their trigonal phase. Using the Li–Ho–Cl components as an example, their structures, phase transition, ionic conductivity, and electrochemical stability are studied. Molecular dynamics simulations reveal the facile diffusion in the z-direction in the orthorhombic structure, rationalizing the improved ionic conductivities. All-solid-state batteries of NMC811/Li2.73Ho1.09Cl6/In demonstrate excellent electrochemical performance at both 25 and −10 °C. As relevant to the vast number of isostructural halide electrolytes, the present structure control strategy guides the design of halide superionic conductors.
AB - Understanding the relationship between structure, ionic conductivity, and synthesis is the key to the development of superionic conductors. Here, a series of Li3-3xM1+xCl6 (−0.14 < x ≤ 0.5, M = Tb, Dy, Ho, Y, Er, Tm) solid electrolytes with orthorhombic and trigonal structures are reported. The orthorhombic phase of Li–M–Cl shows an approximately one order of magnitude increase in ionic conductivities when compared to their trigonal phase. Using the Li–Ho–Cl components as an example, their structures, phase transition, ionic conductivity, and electrochemical stability are studied. Molecular dynamics simulations reveal the facile diffusion in the z-direction in the orthorhombic structure, rationalizing the improved ionic conductivities. All-solid-state batteries of NMC811/Li2.73Ho1.09Cl6/In demonstrate excellent electrochemical performance at both 25 and −10 °C. As relevant to the vast number of isostructural halide electrolytes, the present structure control strategy guides the design of halide superionic conductors.
KW - all-solid-state Li batteries
KW - energy storage
KW - halides
KW - solid-state electrolytes
KW - superionic conductors
UR - http://www.scopus.com/inward/record.url?scp=85127594179&partnerID=8YFLogxK
U2 - 10.1002/aenm.202103921
DO - 10.1002/aenm.202103921
M3 - Article
AN - SCOPUS:85127594179
VL - 12
SP - 11
JO - Advanced Energy Materials
JF - Advanced Energy Materials
SN - 1614-6832
IS - 21
M1 - 2103921
ER -
