Improved Single-Ion Conductivity of Polymer Electrolyte via Accelerated Segmental Dynamics
Sheng Zhao, Yiman Zhang, Hoang Pham, Jan‐Michael Y. Carrillo, Bobby G. Sumpter, Jagjit Nanda, Nancy J. Dudney, Tomonori Saito, Alexei P. Sokolov, Pengfei Cao
Abstract
Single-ion conducting polymer electrolytes (SICPEs) have many advantages for solid-state battery applications, while low conductivities remain the bottleneck for their practical applications. Herein, a strategy that can significantly improve the ionic conductivity of SICPEs based on the concept of accelerated segmental dynamics was demonstrated by the evaluation of the thermal property, rheological behavior, morphology analysis, molecular dynamics simulation, and conductivity performance. With both “soft” poly(dimethylsiloxane) (PDMS) backbone and poly(ethylene glycol) (PEG) side chains, the obtained SICPE possesses faster segmental relaxation and higher lithium-ion conductivity. With lithium “transference” number close to unity, the obtained SICPE also shows excellent electrochemical stability against lithium metal electrodes. The clear relationship established between the segmental dynamics of polymer electrolyte and its ionic conductivity should contribute to achieve a solid electrolyte with improved ionic conductivity toward the next-generation solid-state battery.