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

Nathan Dunlap, Jongbeom Kim, Harvey Guthrey, Chun Jiang, Ian Morrissey, Conrad Stoldt, Kyu Oh, Mowafak Al-Jassim, Se-Hee Lee

Research output: Contribution to journalArticlepeer-review

24 Scopus Citations

Abstract

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. 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.

Original languageAmerican English
Article number060522
Number of pages7
JournalJournal of the Electrochemical Society
Volume167
Issue number6
DOIs
StatePublished - 2020

Bibliographical note

Publisher Copyright:
© 2020 The Electrochemical Society ("ECS"). Published on behalf of ECS by IOP Publishing Limited.

NREL Publication Number

  • NREL/JA-5K00-77222

Keywords

  • Li-ion batteries
  • Si-based anodes

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