Interface Design for All-Solid-State Lithium-Sulfur Batteries

Lithium-sulfur batteries (LSBs) are one of the most promising energy storage technologies due to the low cost and high abundance of S. However, polysulfide shuttling and the intrinsically low electronic conductivity of the S cathode pose severe challenges to their commercialization. In this talk, I will discuss potential strategies to mitigate these drawbacks via interface design in an all-solid-state LSB (SSLSB) architecture. Using DFT calculations and machine learning potentials, we show that sulfides are generally the most stable solid electrolytes and buffer layers for SSLSBs. We also demonstrate that the β-Li₃PS₄(100) surface tends to form interfaces with S₈ with 2D channels and lower activation barriers for Li diffusion. Finally, we also discuss a novel sulfur cathode chemistry that is healable via periodic heating and exhibits high electronic conductivity. These advances pave the way to the realization of practical LSBs.