Real-time tracking the Li⁺-ion transition behavior and dynamics in solid Poly(vinyl alcohol)/LiClO₄ electrolytes

To delicately track the Li-ion transport in SPEs under an external electric field (EF) is a big challenge, considering the limitation of most spectroscopic methods to monitor the real-time conformational changes and track the dynamic process. Herein, real-time Li-ion transition behavior and transport dynamics in typical poly(vinyl alcohol)/LiClO₄ electrolytes under an external EF have been studied by combining time-resolved Fourier transform infrared (FTIR) with two-dimensional correlation FTIR spectroscopy. Results show that no migration of Li-ions has been detected when the time scale of the EF loading is at nanosecond (less than 200 ns). However, for the first time, Li-ions have been found to significantly transfer along the EF direction as the time scale enhances to microsecond order of magnitude and the migration period is less than 10 microseconds. The Li⁺ migration in the SPEs under an EF is a complicated process including quasi-periodic dissociation and coordination effects between Li-ion carriers and polymeric chains.