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New Cost-Effective Halide Solid Electrolytes for All-Solid-State Batteries: Mechanochemically Prepared Fe3+-Substituted Li2ZrCl6

New Cost-Effective Halide Solid Electrolytes for All-Solid-State Batteries: Mechanochemically Prepared Fe3+-Substituted Li2ZrCl6
Kwak, HiramHan, DaseulLyoo, JeynePark, JuhyounJung, Sung HooHan, YoonjaeKwon, GihanKim, HansuHong, Seung-TaeNam, Kyung-WanJung, Yoon Seok
DGIST Authors
Kwak, Hiram; Han, Daseul; Lyoo, Jeyne; Park, Juhyoun; Jung, Sung Hoo; Han, Yoonjae; Kwon, Gihan; Kim, Hansu; Hong, Seung-Tae; Nam, Kyung-Wan; Jung, Yoon Seok
Issue Date
Advanced Energy Materials, 11(12), 2003190
Article Type
Article in press
Author Keywords
electrodeshalidesionic conductivitiessolid electrolytessolid-state batteries
X ray absorption spectroscopyZirconium compoundsAliovalent substitutionAll-solid state batteriesElectrochemical performanceInterfacial stabilitiesMechano-chemical methodsOxide solid electrolytesPair distribution functionsRaman spectroscopy measurementsSolid electrolytesAluminum compoundsBall millingChemical stabilityChlorine compoundsCobalt compoundsCost effectivenessDistribution functionsHeat treatmentIron compoundsIron metallographyLithium compoundsLithium metallographyMetal halidesNickel compoundsRare earthsSolid state devicesSolid-State BatteriesSulfur compounds
Owing to the combined advantages of sulfide and oxide solid electrolytes (SEs), that is, mechanical sinterability and excellent (electro)chemical stability, recently emerging halide SEs such as Li3YCl6 are considered to be a game changer for the development of all-solid-state batteries. However, the use of expensive central metals hinders their practical applicability. Herein, a new halide superionic conductors are reported that are free of rare-earth metals: hexagonal close-packed (hcp) Li2ZrCl6 and Fe3+-substituted Li2ZrCl6, derived via a mechanochemical method. Conventional heat treatment yields cubic close-packed monoclinic Li2ZrCl6 with a low Li+ conductivity of 5.7 × 10−6 S cm−1 at 30 °C. In contrast, hcp Li2ZrCl6 with a high Li+ conductivity of 4.0 × 10−4 S cm−1 is derived via ball-milling. More importantly, the aliovalent substitution of Li2ZrCl6 with Fe3+, which is probed by complementary analyses using X-ray diffraction, pair distribution function, X-ray absorption spectroscopy, and Raman spectroscopy measurements, drastically enhances the Li+ conductivity up to ≈1 mS cm−1 for Li2.25Zr0.75Fe0.25Cl6. The superior interfacial stability when using Li2+xZr1−xFexCl6, as compared to that when using conventional Li6PS5Cl, is proved. Furthermore, an excellent electrochemical performance of the all-solid-state batteries is achieved via the combination of Li2ZrCl6 and single-crystalline LiNi0.88Co0.11Al0.01O2. © 2021 Wiley-VCH GmbH
John Wiley and Sons Inc
Related Researcher
  • Author Hong, Seung-Tae Battery Materials Discovery Laboratory
  • Research Interests Magnesium, calcium, and zinc ion batteries; lithium all-solid-state batteries; Inorganic materials discovery; Solid state chemistry; Crystallography; Mg, Ca, Zn 이온 이차전지; 리튬 전고체전지; 신 무기재료 합성; 고체화학; 결정화학
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Department of Energy Science and EngineeringBattery Materials Discovery Laboratory1. Journal Articles

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