Ameliorating the Li-Li₆PS₅Cl Interface Through the Incorporation of an LixSiOy Interlayer using First-Principles DFT Calculations

In order to overcome the inherent safety and longetivity issues experienced by traditional Li-ion batteries, a significant chunk of battery research in the last two decades has been dedicated towards replacing them with ones employing a solid electrolyte. A key step in this transition involves stabilizing the interface between the solid electrolyte and anode made of lithium metal, faced with issues on reactivity,  in order to ensure long-term electrochemical stability, operational safety, and cycling performance. Using first principles DFT calculations, a novel analysis to the Li-Li₆PS₅Cl interface, based on in situ research involving the use of an LixSiOy amphiphilic layer, is explored. Here, feedback on parameters such as density of states, band-alignment, work-function, and interfacial energy is provided in regards to the adjustment of Li-O mole ratios in the interlayer.