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Towards the Commercialization of the All-Solid-State Li-ion Battery: Local Bonding Structure and the Reversibility of Sheet-Style Si-PAN Anodes

Journal Article · · Journal of the Electrochemical Society (Online)

A slurry-coated sheet-style Si-based anode is developed for use in all-solid-state Li-ion batteries. Inexpensive, mixed-conducting polyacrylonitrile (PAN) is utilized as both binder and conductive additive, enabling Si-rich electrodes (70 wt%) to attain large reversible capacities ~1,500 mAh g-1 (Si) at 1 C rates (>3 mA cm-2). Cross sectional analysis of a discharged all-solid-state half-cell indicates that the Si-PAN anode achieves the largest volumetric specific capacity ever reported for a Li-ion electrode (>1500 mAh cm-3). Ex situ Raman spectroscopic studies reveal that the anodes' reversibility is attributed to the preservation of small tetrahedrally coordinated clusters within their Si nanoparticles upon discharge. We therefore argue that careful lithiation limitations should be implemented in all Si-based Li-ion anodes to preserve this local tetrahedral atomic structure. Furthermore, the slurry-coated sheet-style Si-PAN anodes have been successfully cycled in all-solid-state full-cells against high-voltage nickel-rich NMC 811 composite cathodes to encourage future commercialization of similar sheet-style all-solid-state designs.

Research Organization:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); Air Force Research Laboratory
Grant/Contract Number:
AC36-08GO28308
OSTI ID:
1660002
Report Number(s):
NREL/JA-5K00-77222; MainId:26168; UUID:f2879dac-a39c-41ec-9fa4-328b7de7c563; MainAdminID:13752
Journal Information:
Journal of the Electrochemical Society (Online), Journal Name: Journal of the Electrochemical Society (Online) Journal Issue: 6 Vol. 167; ISSN 1945-7111
Publisher:
IOP PublishingCopyright Statement
Country of Publication:
United States
Language:
English

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