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Most next-generation batteries, such as LiS and Li–O2 batteries, generally consider use of Li metal as the negative electrode (NE) to greatly increase the energy density compared with conventional Li-ion batteries. However, a serious problem of the Li NE in practical use is Li dendrite growth because of cell short circuits. To solve this problem, the Si NE is a good alternative candidate, but this does not include a Li source as the carrier ion. Therefore, Li pre-doping of Si NE will become important for next-generation batteries. In this study, we prepared Li–naphthalenide (Li–NTL) solutions using Li foil, naphthalene, and 2-methyltetrahydrofuran and examined the effect of Li concentration on the Li alloying behavior. In particular, changes in the solvation structure and equilibrium potential of the Li–NTL solution, and the resulting Li alloying depth of the Si NE were evaluated to clarify the Li alloying mechanism by the Li–NTL solution. A high Li concentration generated a larger amount of the [NTL]2− dianion than the [NTL]•– monoanion radical, and exhibited a lower equilibrium potential (Veq). This led to deeper Li alloying of the Si NE, corresponding to a high pre-doping capacity of 3250 mAh g−1 for a 24 h treatment. Li concentration was found to be important to control the amount of dianion in the Li–NTL solution and determined the depth of Li alloying in Si NE.

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  This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Energy Materials, copyright © 2025 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsaem.4c03286.

Keyword: Si anode, Li predoping, prelithiation, Li-naphthalenide, radical anions, next-generation batteries

Date published: 2025-04-14

Publisher: American Chemical Society (ACS)

Journal:

• ACS Applied Energy Materials (ISSN: 25740962) vol. 8 issue. 7 p. 4370-4378

Funding:

• Amano Institute of Technology FY2024
• Seikei University
• National Institute for Materials Science

Manuscript type: Author's version (Accepted manuscript)

MDR DOI: https://doi.org/10.48505/nims.5428

First published URL: https://doi.org/10.1021/acsaem.4c03286

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Updated at: 2025-04-15 09:58:25 +0900

Published on MDR: 2026-04-02 08:25:58 +0900