Revealing Local Diffusion Dynamics in Hybrid Solid Electrolytes
Shengnan Zhang (TU Delft - RST/Storage of Electrochemical Energy)
Leon Felix Mueller (Student TU Delft)
Laurence Macray (Student TU Delft)
Marnix Wagemaker (TU Delft - RST/Storage of Electrochemical Energy)
Lars Bannenberg (TU Delft - RID/TS/Instrumenten groep)
S. Ganapathy (TU Delft - RID/TS/Instrumenten groep, TU Delft - RST/Storage of Electrochemical Energy)
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Abstract
Hybrid solid electrolytes (HSEs) leverage the benefits of their organic and inorganic components, yet optimizing ion transport and component compatibility requires a deeper understanding of their intricate ion transport mechanisms. Here, macroscopic charge transport is correlated with local lithium (Li)-ion diffusivity in HSEs, using poly(ethylene oxide) (PEO) as matrix and Li6PS5Cl as filler. Solvent- and dry-processing methods were evaluated for their morphological impact on Li-ion transport. Through multiscale solid-state nuclear magnetic resonance analysis, we reveal that the filler enhances local Li-ion diffusivity within the slow polymer segmental dynamics. Phase transitions indicate inhibited crystallization in HSEs, with reduced Li-ion diffusion barriers attributed to enhanced segmental motion and conductive polymer conformations. Relaxometry measurements identify a mobile component unique to the hybrid system at low temperatures, indicating Li-ion transport along polymer-filler interfaces. Comparative analysis shows solvent-processed HSEs exhibit better morphological uniformity and enhanced compatibility with Li-metal anodes via an inorganic-rich solid electrolyte interphase.
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