Transport and mechanical properties of pseudo-zwitterionic polymer electrolytes from non-equilibrium molecular dynamics simulations
Year: 2026
Type: preprint
Abstract: Pseudo-zwitterionic polymer electrolytes (PZPEs) are promising multifunctional copolymers for solid-state batteries, where efficient ion transport must be balanced against mechanical robustness. Here, we used non-equilibrium molecular dynamics (NEMD) simulations to determine how polymer composition, LiTFSI concentration, and copolymer sequence govern coupled transport and mechanical properties in MIL:PEGMbased PZPEs. A calibrated field-driven NEMD protocol enables ionic conductivity to be obtained within a few nanoseconds while preserving the equilibrium salt-concentration dependence. It is found that Li+ self-diffusion decreases with increasing salt concentration in PEGM-rich systems but can increase in MIL-rich systems, accompanied by a shift toward TFSI− rich coordination. Onsager analysis further shows that cation–anion correlations strongly influence electrophoretic mobility. The resulting conductivity–modulus maps reveal a clear trade-off: PEGM-rich systems are more conductive but softer, whereas MIL-rich systems are stiffer but less conductive. NEMD simulations suggest that salt concentration and copolymer sequence provide additional handles for tuning this balance.
Source: ChemRxiv
Language: English
Subfield: Electrical and Electronic Engineering
Field: Engineering
Domain: Physical Sciences
Open Access status: green
Awards: G2236846416, G4632909464, G5095843378, G54735966, G6129367363, G6523014278, G6830658824, SMART SENSORS AND SELF-HEALING FUNCTIONALITIES EMBEDDED FOR BATTERY LONGEVITY WITH MANUFACTURABILITY AND ECONOMICAL RECYCLABILITY, BATTERY 2030+ CSA3 large-scale research initiative: At the heart of a connected green society, NAISS
OpenAlex ID: W7213976574