Journal Article

FZJ-2022-03450

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Forced Disorder in the Solid Solution Li3P–Li2S: A New Class of Fully Reduced Solid Electrolytes for Lithium Metal Anodes

Szczuka, C.FZJ* ; Karasulu, B. ; Groh, M. F. ; Sayed, F. N. ; Sherman, T. J. ; Bocarsly, J. D. ; Vema, S. ; Menkin, S. ; Emge, S. P. ; Morris, A. J. ; Grey, C. P. (Corresponding author)

2022
American Chemical Society Washington, DC

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Please use a persistent id in citations: http://hdl.handle.net/2128/31887  doi:10.1021/jacs.2c01913

Abstract: All-solid-state batteries based on non-combustible solid electrolytes are promising candidates for safe energy storage systems. In addition, they offer the opportunity to utilize metallic lithium as an anode. However, it has proven to be a challenge to design an electrolyte that combines high ionic conductivity and processability with thermodynamic stability toward lithium. Herein, we report a new highly conducting solid solution that offers a route to overcome these challenges. The Li–P–S ternary was first explored via a combination of high-throughput crystal structure predictions and solid-state synthesis (via ball milling) of the most promising compositions, specifically, phases within the Li3P–Li2S tie line. We systematically characterized the structural properties and Li-ion mobility of the resulting materials by X-ray and neutron diffraction, solid-state nuclear magnetic resonance spectroscopy (relaxometry), and electrochemical impedance spectroscopy. A Li3P–Li2S metastable solid solution was identified, with the phases adopting the fluorite (Li2S) structure with P substituting for S and the extra Li+ ions occupying the octahedral voids and contributing to the ionic transport. The analysis of the experimental data is supported by extensive quantum-chemical calculations of both structural stability, diffusivity, and activation barriers for Li+ transport. The new solid electrolytes show Li-ion conductivities in the range of established materials, while their composition guarantees thermodynamic stability toward lithium metal anodes.

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Contributing Institute(s):

1. Grundlagen der Elektrochemie (IEK-9)

Research Program(s):

1. 1223 - Batteries in Application (POF4-122) (POF4-122)

Appears in the scientific report 2022

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