4.8 Article

Achieving a high loading of cathode in PVDF-based solid-state battery

Journal

ENERGY & ENVIRONMENTAL SCIENCE
Volume 17, Issue 1, Pages 344-353

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d3ee03108j

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The lack of understanding of ion transport in the cathode of PVDF-based solid-state lithium metal batteries limits their performance. The use of carbon-coated Li1.4Al0.4Ti1.6(PO4)3 nanowires as a cathode filler improves the diffusion of ions in the thick cathode, leading to enhanced battery performance and stability.
The lack of fundamental understanding of ion transport in the cathode of polyvinylidene fluoride (PVDF)-based solid-state lithium metal batteries restricts their rate performance and cycle stability, especially under high cathode mass loadings. Herein, we reveal that the lithium ion (Li+) solvated with N,N-dimethylformamide ([Li(DMF)x]+) in PVDF electrolyte spontaneously diffuses into the cathode, but its diffusion depth is limited, and a continuous Li+ transport network can only be built in cathodes with low loadings. We further find that carbon-coated Li1.4Al0.4Ti1.6(PO4)3 nanowires (C@LATP NW) as a cathode filler not only conduct Li+, but also exhibit strong adsorption of the [Li(DMF)x]+ complex, which promotes the uniform diffusion of [Li(DMF)x]+ in a thick cathode to construct a highly efficient Li+ transport network and achieve full reaction of the thick cathode. The carbon layer on C@LATP NW greatly suppresses the side decomposition reactions of DMF and LiFSI to improve the stability of the conductive network and structure of the cathode materials. The cathode with 3 wt% C@LATP NW enables excellent rate performance and cycle stability of solid-state batteries with high mass loadings of up to 15 mg cm-2, which opens a way for practical cathode design of solid-state batteries. We construct an efficient Li+ transport network in a high loading cathode using carbon coated Li1.4Al0.4Ti1.6(PO4)3 nanowires, which has a strong adsorption for [Li(DMF)x]+ of PVDF-based SPEs to promote its uniform diffusion and stability in cathode.

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