Ion Clusters and Networks in Water-in-Salt Electrolytes

Water-in-salt electrolytes (WiSEs) are a class of super-concentrated that have shown much promise in replacing organic lithium-ion batteries. At the extremely high salt concentrations WiSEs, ionic association is more complicated than simple ion pair description. In fact, large branched clusters can be present and past critical concentration, an infinite percolating network form spontaneously. this work, we simplify our recently developed thermodynamic model reversible aggregation gelation, tailoring it specifically for WiSEs. Our simplified theory only has handful parameters, all which readily determined from simulations. able to quantitatively reproduce populations different sizes as function concentration fraction ions incorporated into gel, observed molecular simulations three lithium-based The extent gelation greatly affects effective strength solution, coordination environment active cations known govern chemistry solid-electrolyte interface, activity species electrolyte.