Plasticized Hybrid Network Solid Polymer Electrolytes for Lithium‐Metal Batteries

Abstract

Incorporating solid polymer electrolyte (SPE) into lithium metal batteries has the benefit of employing the electrolyte as the electrode separator while inhibiting the growth of lithium dendrites. The two main models on lithium dendrite growth show that either ionic conductivity or mechanical property affect lithium dendrite nucleation and growth rate. In this work, with a well‐controlled hybrid network SPE as the model system, the modulus and conductivity of the hybrid SPEs are systematically tuned by plasticizing the network with low molecular with diluents. This systematic property control allows for establishing the correlation between mechanical/electrochemical properties of the SPEs with their propensity of lithium dendrite resistance using galvanostatic polarization and cycling experiments. It is further demonstrated that lithium metal batteries can be operated at 30 °C for the plasticized SPEs due to the dramatically improved conductivity.

Thiol‐Branched Solid Polymer Electrolyte Featuring High Strength, Toughness, and Lithium Ionic Conductivity for Lithium‐Metal Batteries

“…Such a combination of high strains and high tensile deformation should be helpful to inhibit the growth of lithium dendrites. [ 24,36 ] It is also worthwhile noting that M‐S‐PEGDA has a much higher strength and strain capacity than conventional PEO‐based polymer electrolytes (Figure 2d), [ 26,27,37–48 ] indicating promising application prospects in all‐solid‐state LMBs to endure long periods of charge/discharge cycles.…”

Concentration polarization and metal dendrite initiation in isolated electrolyte microchannels

“…In contrast, polymer electrolytes without inert porous structures were found to yield scaling exponents close to -2 between the cumulative time before penetration and the cycling current density. [57][58][59][60] The exact value of -2 was reported by Schaefer et al 61 from cells using a freestanding gel-type electrolyte, but with SiO2 nanoparticles. The volume fraction of the nanoparticles was controlled to be 0.15, much lower than the inert volume fraction (0.6) of typical porous separators with porosity around 0.4.…”

High ionic conduction, toughness and self-healing poly(ionic liquid)-based electrolytes enabled by synergy between flexible units and counteranions

“…It is also worthwhile noting that PIL-BA 50 TFSI has much higher strain capacity and ionic conductivity than most reported polymer electrolytes (Fig. 6f), [34][35][36][37][38][39][40][41][42][43][44][45][46][47] indicating promising application prospects in all-solid-state electrochemical devices to ensure high security during the long-term cycles.…”