Issue 46, 2017

An insight into intrinsic interfacial properties between Li metals and Li10GeP2S12 solid electrolytes

Abstract

Density functional theory simulations and experimental studies were performed to investigate the interfacial properties, including lithium ion migration kinetics, between lithium metal anode and solid electrolyte Li10GeP2S12(LGPS). The LGPS[001] plane was chosen as the studied surface because the easiest Li+ migration pathway is along this direction. The electronic structure of the surface states indicated that the electrochemical stability was reduced at both the PS4- and GeS4-teminated surfaces. For the interface cases, the equilibrium interfacial structures of lithium metal against the PS4-terminated LGPS[001] surface (Li/PS4–LGPS) and the GeS4-terminated LGPS[001] surface (Li/GeS4–LGPS) were revealed based on the structural relaxation and adhesion energy analysis. Solid electrolyte interphases were expected to be formed at both Li/PS4–LGPS and Li/GeS4–LGPS interfaces, resulting in an unstable state of interface and large interfacial resistance, which was verified by the EIS results of the Li/LGPS/Li cell. In addition, the simulations of the migration kinetics show that the energy barriers for Li+ crossing the Li/GeS4–LGPS interface were relatively low compared with the Li/PS4–LGPS interface. This may contribute to the formation of Ge-rich phases at the Li/LGPS interface, which can tune the interfacial structures to improve the ionic conductivity for future all-solid-state batteries. This work will offer a thorough understanding of the Li/LGPS interface, including local structures, electronic states and Li+ diffusion behaviors in all-solid-state batteries.

Graphical abstract: An insight into intrinsic interfacial properties between Li metals and Li10GeP2S12 solid electrolytes

Supplementary files

Article information

Article type
Paper
Submitted
03 Aug 2017
Accepted
08 Nov 2017
First published
08 Nov 2017

Phys. Chem. Chem. Phys., 2017,19, 31436-31442

An insight into intrinsic interfacial properties between Li metals and Li10GeP2S12 solid electrolytes

B. Chen, J. Ju, J. Ma, J. Zhang, R. Xiao, G. Cui and L. Chen, Phys. Chem. Chem. Phys., 2017, 19, 31436 DOI: 10.1039/C7CP05253G

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