Authors
Jian-Fen Wang, Matthias Weiling, Felix Pfeiffer, Marian C Stan, Martin Winter, Masoud Baghernejad
Published in
Advanced science (Weinheim, Baden-Wurttemberg, Germany). Pages e77788. Sep 16, 2026. Epub Sep 16, 2026.
Abstract
Polycaprolactones (PCL) have gained attention as a biodegradable and environmentally sustainable solid polymer electrolyte (SPE) for solid-state battery applications. While poly(ethylene oxide) (PEO) systems are widely studied, the interfacial mechanisms of PCL-based SPEs in contact with Li metal remain insufficiently explored. In this work, operando attenuated total reflection Fourier-transform infrared (ATR-FTIR) spectroscopy was employed to monitor the chemical environment at the interface of Li metal and crosslinked PCL-based SPEs (cl-PCL5LiTFSI) during Li plating/stripping, enabling both spectral assignment and electrochemical comparison between the crosslinked and non-crosslinked systems. During galvanostatic cycling experiments, cells with cl-PCL5LiTFSI SPEs exhibited increased cycling stability compared to cells containing PCL5LiTFSI SPEs, which can be attributed to the enhanced mechanical strength of the polymer network. Overall, the results show the development of localized ordered PCL domains and the redistribution of TFSI- anion during Li plating/stripping, revealing the possible degradation and dynamic changes occurring at the SPE|Li metal interface. The phenomenon of interfacial evolution of the SPEs was visualized through converting specific characteristic bands of PCL and LiTFSI from operando spectra into penetration depth-dependent band ratio maps.
PMID:
42750247
Bibliographic data and abstract were imported from PubMed on 17 Sep 2026.
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