Design of a unique anion framework in halospinels for outstanding performance of all solid-state Li-ion batteries: first-principles approach

Hoje Chun, Kyungju Nam, Sung Jun Hong, Joonhee Kang, Byungchan Han

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9 Citations (Scopus)


A solid-state electrolyte (SSE) is a key component in the performance control of all-solid-state Li-ion batteries. The development of a promising material has, however, come to a standstill due to the undesirably low ionic conductivity and stability. Using first-principles calculations, we propose that halospinels,i.e., Li2Sc2/3X4(X = Cl, Br, and I), should be encouraging materials to surmount the long-standing challenges. Density functional theory (DFT) calculations unveil their underlying mechanisms that the incorporated halogen anion and Sc form unique ionic pairs to create the atomic environment required for the dramatic facilitation of Li-ion diffusion to a superionic conductor level. In addition, collective ionic motions near the halogen species in the halospinel solid electrolyte promote the substantial enhancement of the electrochemical stability and interface compatibility with the electrodes. We demonstrate that a crucial factor is the rational selection of the halogen anion to achieve the maximal performance of the electrolyte.Ab initiomolecular dynamics (AIMD) simulations consistently pinpoint that the halospinel with Cl anion, Li2Sc2/3Cl4, is the best choice to maintain the high functionality of Li-ion conductivity, electrochemical stability, and interface compatibility with the LiCoO2electrode in Li-ion battery applications. Our study provides a fundamental ground on chemical design principles for a breakthrough in advancing solid-state electrolytes towards a wide commercialization of all-solid-state Li-ion batteries.

Original languageEnglish
Pages (from-to)15605-15612
Number of pages8
JournalJournal of Materials Chemistry A
Issue number28
Publication statusPublished - 2021 Jul 28

Bibliographical note

Funding Information:
This work was supported by the Global Frontier Program through the Global Frontier Hybrid Interface Materials (GFHIM) of the NRF funded by the Ministry of Science and ICT (project no. 2013M3A6B1078882) and by the Research and Development Program of KIER (C1-2447) in the Republic of Korea.

Publisher Copyright:
© The Royal Society of Chemistry 2021.

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Renewable Energy, Sustainability and the Environment
  • Materials Science(all)


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