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Issue 8, 2021

Two-dimensional materials as a stabilized interphase for the solid-state electrolyte Li10GeP2S12 in lithium metal batteries

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Abstract

Superionic conductor Li10GeP2S12 has a high lithium-ion conductivity of 12 mS cm−1 at room temperature, but its poor chemical stability against lithium metal anodes restricts its practical use. Introducing suitable two-dimensional (2D) sheets between Li10GeP2S12 and a lithium metal anode as a solid-electrolyte interphase (SEI) is expected to solve the interfacial problem without sacrificing energy density. A set of systematic selection schemes for 2D SEIs involving thermodynamic, electronic, and mechanical properties is proposed. h-BN and α-BNyne are finally selected, and first-principles calculations are carefully performed. Compared with the case where Li10GeP2S12 is directly exposed to a lithium metal anode, the two interfaces added by the ultrathin h-BN or α-BNyne monolayer as a SEI become chemically stabilized, with the electrochemical windows expanded by 2.08–2.41 eV. Significantly higher and wider barriers for electrons form while maintaining acceptable Li-ion diffusion barriers at the interfaces. The simple theoretical 2D SEI screening scheme exhibited here can be extended to other solid-state battery systems.

Graphical abstract: Two-dimensional materials as a stabilized interphase for the solid-state electrolyte Li10GeP2S12 in lithium metal batteries

Supplementary files

Article information


Submitted
03 Aug 2020
Accepted
11 Jan 2021
First published
11 Jan 2021

J. Mater. Chem. A, 2021,9, 4810-4821
Article type
Paper

Two-dimensional materials as a stabilized interphase for the solid-state electrolyte Li10GeP2S12 in lithium metal batteries

J. Ma, R. Quhe, Z. Zhang, C. Yang, X. Zhang, J. Li, L. Xu, J. Yang, B. Shi, S. Liu, L. Xu, X. Sun and J. Lu, J. Mater. Chem. A, 2021, 9, 4810 DOI: 10.1039/D0TA07589B

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