Unveiling Interfacial Li-Ion Dynamics in Li₇La₃Zr₂O₁₂/PEO(LiTFSI) Composite Polymer-Ceramic Solid Electrolytes for All-Solid-State Lithium Batteries

Unlocking the full potential of solid-state electrolytes (SSEs) is key to enabling safer and more-energy dense technologies than today's Li-ion batteries. In particular, composite materials comprising a conductive, flexible polymer matrix embedding ceramic filler particles are emerging as good strategy provide combination conductivity mechanical chemical stability demanded from SSEs. However, electrochemical activity these strongly depends on their polymer/ceramic interfacial dynamics at molecular scale, whose fundamental understanding remains elusive. While this interface has been explored for nonconductive fillers, atomistic modeling interfaces involving potentially more promising conductive still lacking. We address shortfall by employing enhanced Monte Carlo techniques gain unprecedented insights into in polymer-ceramic electrolyte, which integrates polyethylene oxide plus LiN(CF3SO2)2 lithium imide salt (LiTFSI), cubic Li7La3Zr2O12 (LLZO) inclusions. Our simulations automatically produce distribution assumed space-charge models and, first time, long-range impact garnet surface diffusivity unveiled. Based our calculations experimental measurements tensile strength ionic conductivity, we able explain previously reported drop critical fraction well below theoretical percolation threshold. results pave way computational other filler/polymer combinations rational design