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Composite polymer electrolytes (CPEs), consisting of solid electrolyte particles embedded within a solid polymer electrolyte matrix, are promising materials for all-solid-state batteries due to their mechanical properties and scalable production process. In this study, CPEs consisting of
LiTFSI blended with 1 wt%, 10 wt% and 40 wt% (CPE40) of LiPSCl electrolyte filler are prepared by a slurry-based process. The incorporation of LiPSCl improves the lithium ion conductivity from 0.84 mS cm (
LiTFSI) to 3.6 mS cm (CPE40) at 80 °C. Surface-sensitive X-ray photoelectron spectroscopy reveals LiF, polysulfides and LiPO on the CPE surface, originating from decomposition reactions between
LiTFSI and LiPSCl. The decomposition products influence the formation of the solid electrolyte interphase (SEI) at the lithium metal | CPE interface, resulting in a reduced SEI resistance of 3.3 Ω cm (CPE40) compared to 5.8 Ω cm (
LiTFSI) at 80 °C. The SEI growth follows a parabolic rate law and the growth rate declines from 1.2 Ω cm h (
LiTFSI) to 0.57 Ω cm h (CPE40) during thermal aging at 80 °C. By substituting CPEs for SPEs in lithium plating and stripping experiments, the increase in SEI resistance was reduced by more than 75%. In order to get a deeper understanding of the SEI formation process, in situ XPS measurements were carried out where lithium metal is successively deposited on the CPE sample and X-ray photoelectron spectroscopy is measured after each deposition step. On the basis of these measurements, a multistep decomposition mechanism is postulated, including the formation of LiF and LiS as key components of the SEI.
This article was published in the following journal.
Name: ACS applied materials & interfaces
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