Article Mechanistic insight of Li cluster formation and dendrite deposition in sulfide all-solid-state battery with hard-carbon electrode analyzed using 7Li operando nuclear magnetic resonance

Osamu Tagami ; Hibiki Fukushima ; Yumu Nishigaki ; Ayumi Shikata ORCID ; Masakuni Takahashi ; Kenjiro Hashi SAMURAI ORCID ; Shinobu Ohki SAMURAI ORCID ; Takashi Teranishi ORCID ; Kazuma Gotoh ORCID

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Citation
Osamu Tagami, Hibiki Fukushima, Yumu Nishigaki, Ayumi Shikata, Masakuni Takahashi, Kenjiro Hashi, Shinobu Ohki, Takashi Teranishi, Kazuma Gotoh. Mechanistic insight of Li cluster formation and dendrite deposition in sulfide all-solid-state battery with hard-carbon electrode analyzed using 7Li operando nuclear magnetic resonance. Journal of Power Sources. 2025, 662 (), 238755. https://doi.org/10.1016/j.jpowsour.2025.238755

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(abstract)

Because lithium dendrite deposition during charging and discharging of all solid-state batteries (ASSLBs) is an important difficulty leading to deactivation, precise analysis of the lithium state is indispensable. We explored the potential use of hard-carbon (HC) for an ASSLB anode using operando 7Li NMR to investigate lithium behavior. Cells using circular electrodes capable of applying constraint pressure to the electrode material were fabricated to achieve precise operando NMR measurements for sulfur-based ASSLBs. Adsorption and desorption behaviors of lithium in HC were found to be nearly identical to those of HC in liquid LIBs. However, short circuits occurred after several hours of constant current overlithiation or potential holding at −5.5 mV although no clear amplification of Li dendrite signal was observed. Signal components attributable to quasimetallic clusters were observed in both cases, which suggests that lithium can form clusters in open pores or on the HC surface during overlithiation. Clusters in the open pores or surface can conduct electricity and may serve as nucleation sites for dendrite growth. Although the use of HC anodes can suppress dendrite formation in ASSLBs, more precise voltage control is required than that used for liquid LIBs.

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Keyword: operand nmr

Date published: 2025-11-07

Publisher: Elsevier BV

Journal:

  • Journal of Power Sources (ISSN: 03787753) vol. 662 238755

Funding:

  • American Theological Library Association JPJ004596
  • Japan Society for the Promotion of Science 23K04535

Manuscript type: Publisher's version (Version of record)

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First published URL: https://doi.org/10.1016/j.jpowsour.2025.238755

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Updated at: 2026-01-09 10:15:02 +0900

Published on MDR: 2026-01-09 12:22:32 +0900

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