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Anionic Sublattices in Halide Solid Electrolytes: A Case Study with the High-Pressure Phase of Li3ScCl6.
Ding, Fenghua; Doi, Atsunori; Ogawa, Takafumi; Ubukata, Hiroki; Zhu, Tong; Kato, Daichi; Tassel, Cédric; Oikawa, Itaru; Inui, Naoki; Kuze, Satoru; Yamabayashi, Tsutomu; Fujii, Kotaro; Yashima, Masatomo; Ou, Xing; Wang, Zhijian; Min, Xiaobo; Fujita, Koji; Takamura, Hitoshi; Kuwabara, Akihide; Zhang, Tianren; Griffith, Kent J; Lin, Zhang; Chai, Liyuan; Kageyama, Hiroshi.
Afiliação
  • Ding F; Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University Nishikyo-ku, Kyoto, 615-8510, Japan.
  • Doi A; Advanced Materials Development Laboratory, Sumitomo Chemical Co. Ltd., Tsukuba, 300-3294, Japan.
  • Ogawa T; Nanostructures Research Laboratory, Japan Fine Ceramics Center, Nagoya, 456-8587, Japan.
  • Ubukata H; Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University Nishikyo-ku, Kyoto, 615-8510, Japan.
  • Zhu T; Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University Nishikyo-ku, Kyoto, 615-8510, Japan.
  • Kato D; Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University Nishikyo-ku, Kyoto, 615-8510, Japan.
  • Tassel C; Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University Nishikyo-ku, Kyoto, 615-8510, Japan.
  • Oikawa I; Department of Materials Science, Graduate School of Engineering, Tohoku University, Sendai, 980-8579, Japan.
  • Inui N; Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University Nishikyo-ku, Kyoto, 615-8510, Japan.
  • Kuze S; Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University Nishikyo-ku, Kyoto, 615-8510, Japan.
  • Yamabayashi T; Energy & Functional Materials Research Laboratory, Sumitomo Chemical Co. Ltd., Niihama, 792-8521, Japan.
  • Fujii K; Department of Chemistry, School of Science, Tokyo Institute of Technology, 2-12-1-W4-17, O-okayama, Meguro-ku, Tokyo, 152-8551, Japan.
  • Yashima M; Department of Chemistry, School of Science, Tokyo Institute of Technology, 2-12-1-W4-17, O-okayama, Meguro-ku, Tokyo, 152-8551, Japan.
  • Ou X; School of Metallurgy and Environment, Central South University, Changsha, 410083, PR China.
  • Wang Z; Hunan Rare Earth Metal Materials Research Institute Co. Ltd., Changsha, 410126, PR China.
  • Min X; School of Metallurgy and Environment, Central South University, Changsha, 410083, PR China.
  • Fujita K; Department of Material Chemistry, Graduate School of Engineering, Kyoto, University, Nishikyo-ku, Kyoto, 615-8510, Japan.
  • Takamura H; Department of Materials Science, Graduate School of Engineering, Tohoku University, Sendai, 980-8579, Japan.
  • Kuwabara A; Nanostructures Research Laboratory, Japan Fine Ceramics Center, Nagoya, 456-8587, Japan.
  • Zhang T; Department of Chemistry & Biochemistry, University of California, San Diego, La Jolla, California, 92093, USA.
  • Griffith KJ; Department of Chemistry & Biochemistry, University of California, San Diego, La Jolla, California, 92093, USA.
  • Lin Z; School of Metallurgy and Environment, Central South University, Changsha, 410083, PR China.
  • Chai L; School of Metallurgy and Environment, Central South University, Changsha, 410083, PR China.
  • Kageyama H; Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University Nishikyo-ku, Kyoto, 615-8510, Japan.
Angew Chem Int Ed Engl ; 63(15): e202401779, 2024 Apr 08.
Article em En | MEDLINE | ID: mdl-38363076
ABSTRACT
The Li3MX6 compounds (M=Sc, Y, In; X=Cl, Br) are known as promising ionic conductors due to their compatibility with typical metal oxide cathode materials. In this study, we have successfully synthesized γ-Li3ScCl6 using high pressure for the first time in this family. Structural analysis revealed that the high-pressure polymorph crystallizes in the polar and chiral space group P63mc with hexagonal close-packing (hcp) of anions, unlike the ambient-pressure α-Li3ScCl6 and its spinel analog with cubic closed packing (ccp) of anions. Investigation of the known Li3MX6 family further revealed that the cation/anion radius ratio, rM/rX, is the factor that determines which anion sublattice is formed and that in γ-Li3ScCl6, the difference in compressibility between Sc and Cl exceeds the ccp rM/rX threshold under pressure, enabling the ccp-to-hcp conversion. Electrochemical tests of γ-Li3ScCl6 demonstrate improved electrochemical reduction stability. These findings open up new avenues and design principles for lithium solid electrolytes, enabling routes for materials exploration and tuning electrochemical stability without compositional changes or the use of coatings.
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Texto completo: 1 Base de dados: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Ano de publicação: 2024 Tipo de documento: Article País de afiliação: Japão
Texto completo
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PubMed Links
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Texto completo: 1 Base de dados: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Ano de publicação: 2024 Tipo de documento: Article País de afiliação: Japão