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Page 12 of 35 Tao et al. Energy Mater 2022;2:200036 https://dx.doi.org/10.20517/energymater.2022.46

Figure 8. Open-circuit energy diagrams of various cell systems. (A) Overall illustration of a cell consisting of a liquid electrolyte (mc and
ma represent the energy levels of the cathode and anode materials, respectively, HOMO and LUMO refer to the highest occupied and
lowest unoccupied molecular orbitals of the liquid electrolyte, respectively, C.B. and V.B. represent the conduction and valence bands of
the SSE, respectively, and Voc represents the open-circuit voltage of the cell). (B) Stable energy window related to liquid electrolyte and
(C) SSE (reproduced with permission from [87,88] ).

investigation and understanding of the interfaces in ASSLSBs require computational methods to effectively
predict and reveal the interfacial stability properties because most direct experimental detecting techniques
easily destroy the solid/solid interfaces in the separation process of samples.

COMPUTATIONAL PREDICTION OF INTERFACIAL STABILITY BETWEEN ELECTRODES
AND SSES
Owing to their high-throughput nature, several computational methods, including density functional theory
and ab initio molecular dynamics simulations, have been employed to identify the theoretical/intrinsic
formation of interfaces, confirm the existence of space-charge layers and analyze the possible interfacial
reactions in a working cell. The stability of electrode/electrolyte interfaces at various levels can be evaluated
systematically [89-92] .

Cathode side
For both conventional liquid electrolyte-based LSBs and ASSLSBs, conductive host materials are an integral
part of S-based cathodes due to the insulating nature of S and lithium sulfide. In various types of host