Publication date: 10th April 2024
By replacing organic electrolyte solutions with a solid inorganic equivalent, all solid-state batteries (ASSBs) can potentially mitigate the safety issues known for conventional Li-ion batteries, and provide enhanced energy densities when coupled with the Li metal, the ultimate Li-ion anode. Mechanical and (electro)chemical incompatibilities between the ASSB solid components, however, lead to high resistances, curtailing the Li-ion transport at their interfaces.
In this talk, I will introduce a high-throughput modelling approach based on first principles and machine-learning potentials to explore novel ASSB materials with superior features as well as to rationally design more stable interfaces between ASSB components using our automated interface generation code (INTERFACER). I will also elaborate on a specific application that lead to the discovery of a new class of solid Li-P-S electrolytes, Li2S─Li3P solid solutions, which are intrinsically stable electrochemically against the Li metal anodes. I will discuss the mechanisms underlying the higher ionic conductivity and higher electrochemical stability of these new Li-P-S solid solutions as compared to other well-known thiophosphate electrolytes, as revealed by the atomic-level simulations.
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