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The fabrication of all-solid-state batteries using lithium metal that can be operated at high current densities (free lithium dendrites) is a recognized worldwide goal. We used a glassy lithium borate (LBO)–based microstructure as the grain boundary modifier of a garnet-type solid electrolyte to prevent lithium dendrite formation at high current densities. The relative density (90 %) and ionic conductivity (10–4 S cm–1) were similar for LBO-modified and non-modified solid electrolytes. Notably, a post-annealing step at 175 ◦C significantly reduces the interfacial resistance between the LBO-modified electrolyte and lithium metal. LBO in the solid electrolyte microstructure distributes the current and prevents dendrite propagation, suppressing lithium dendrites up to 10 mA cm–2. Low voltage response at a current density of 10 mA cm–2 for 60 galvanostatic plating–stripping cycles establishes the fast-charging capability of this composite electrolyte. Density functional theory calculations reveal that LBO offers a broader electrochemical stability window compared to LLZ, enhancing overall stability within the 0–3.4 V range. This work provides a promising route to simultaneously achieve high current density operation and improved interfacial stability in garnet-based solid-state batteries, accelerating the practical implementation of lithium-metal anodes.

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• Creative Commons BY-NC-ND Attribution-NonCommercial-NoDerivs 4.0 International
  

Keyword: all solid state batteries, garnet solid electrolytes, lithium dendrites, Li2O-B2O3, critical current density, density functional theory methods

Date published: 2025-04-16

Publisher: Elsevier BV

Journal:

• Electrochimica Acta (ISSN: 00134686) vol. 528 146233

Funding:

• Nippon Sheet Glass Foundation for Materials Science and Engineering
• Ministry of Science, Technology, and Innovation of Colombia "Minciencias"

Manuscript type: Author's version (Accepted manuscript)

MDR DOI: https://doi.org/10.48505/nims.5742

First published URL: https://doi.org/10.1016/j.electacta.2025.146233

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Updated at: 2025-09-10 08:30:31 +0900

Published on MDR: 2025-09-10 08:22:24 +0900