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Overcoming low initial coulombic efficiencies of Si anodes through prelithiation in all-solid-state batteries.

ABSTRACT: All-solid-state batteries using Si as the anode have shown promising performance without continual solid-electrolyte interface (SEI) growth. However, the first cycle irreversible capacity loss yields low initial Coulombic efficiency (ICE) of Si, limiting the energy density. To address this, we adopt a prelithiation strategy to increase ICE and conductivity of all-solid-state Si cells. A significant increase in ICE is observed for Li₁Si anode paired with a lithium cobalt oxide (LCO) cathode. Additionally, a comparison with lithium nickel manganese cobalt oxide (NCM) reveals that performance improvements with Si prelithiation is only applicable for full cells dominated by high anode irreversibility. With this prelithiation strategy, 15% improvement in capacity retention is achieved after 1000 cycles compared to a pure Si. With Li₁Si, a high areal capacity of up to 10 mAh cm^-2 is attained using a dry-processed LCO cathode film, suggesting that the prelithiation method may be suitable for high-loading next-generation all-solid-state batteries.

SUBMITTER: Ham SY

PROVIDER: S-EPMC10998844 | biostudies-literature | 2024 Apr

REPOSITORIES: biostudies-literature

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Overcoming low initial coulombic efficiencies of Si anodes through prelithiation in all-solid-state batteries.

Ham So-Yeon SY Sebti Elias E Cronk Ashley A Pennebaker Tyler T Deysher Grayson G Chen Yu-Ting YT Oh Jin An Sam JAS Lee Jeong Beom JB Song Min Sang MS Ridley Phillip P Tan Darren H S DHS Clément Raphaële J RJ Jang Jihyun J Meng Ying Shirley YS

Nature communications 20240406 1

All-solid-state batteries using Si as the anode have shown promising performance without continual solid-electrolyte interface (SEI) growth. However, the first cycle irreversible capacity loss yields low initial Coulombic efficiency (ICE) of Si, limiting the energy density. To address this, we adopt a prelithiation strategy to increase ICE and conductivity of all-solid-state Si cells. A significant increase in ICE is observed for Li<sub>1</sub>Si anode paired with a lithium cobalt oxide (LCO) ca ...[more]

PMID: 38582753

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Project description:HighlightsThe chemical process of local oxidation-partial reduction-deep coupling for stibnite reduction of carbon dots (CDs) is revealed by in-situ high-temperature X-ray diffraction. Sb2S3@xCDs anode delivers high initial coulombic efficiency in lithium ion batteries (85.2%) and sodium ion batteries (82.9%), respectively. C-S bond influenced by oxygen-rich carbon matrix can restrain the conversion of sulfur to sulfite, well confirmed by X-ray photoelectron spectroscopy characterization of solid electrolyte interphase layers helped with density functional theory calculations. CDs-induced Sb-O-C bond is proved to effectively regulate the interfacial electronic structure. The application of Sb2S3 with marvelous theoretical capacity for alkali metal-ion batteries is seriously limited by its poor electrical conductivity and low initial coulombic efficiency (ICE). In this work, natural stibnite modified by carbon dots (Sb2S3@xCDs) is elaborately designed with high ICE. Greatly, chemical processes of local oxidation-partial reduction-deep coupling for stibnite reduction of CDs are clearly demonstrated, confirmed with in situ high-temperature X-ray diffraction. More impressively, the ICE for lithium-ion batteries (LIBs) is enhanced to 85%, through the effect of oxygen-rich carbon matrix on C-S bonds which inhibit the conversion of sulfur to sulfite, well supported by X-ray photoelectron spectroscopy characterization of solid electrolyte interphase layers helped with density functional theory calculations. Not than less, it is found that Sb-O-C bonds existed in the interface effectively promote the electronic conductivity and expedite ion transmission by reducing the bandgap and restraining the slip of the dislocation. As a result, the optimal sample delivers a tremendous reversible capacity of 660 mAh g-1 in LIBs at a high current rate of 5 A g-1. This work provides a new methodology for enhancing the electrochemical energy storage performance of metal sulfides, especially for improving the ICE.

Dataset Information

Overcoming low initial coulombic efficiencies of Si anodes through prelithiation in all-solid-state batteries.

Publications

Overcoming low initial coulombic efficiencies of Si anodes through prelithiation in all-solid-state batteries.

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