Journal
INORGANIC CHEMISTRY
Volume 61, Issue 30, Pages 11746-11756Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.2c01439
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Funding
- Japan Society of the Promotion of Science (JSPS) KAKENHI [JP16H06440, JP17K19172, JP18H01892, JP19H00883, JP21K19027, JP21H05568, JP21K20489, JP21H04619]
- Murata Science Foundation and Collaborative Research Project of Laboratory for Materials and Structures, Institute of Innovative Research, Tokyo Institute of Technology
- Collaborative Research Project of Laboratory for Materials and Structures, Institute of Innovative Research, Tokyo Institute of Technol-ogy
- JST, PRESTO, Japan [JPMJPR21QB]
- SAGA-LS Advisory Committee
- Research Institute for Information Technology, Kyushu University
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A novel perovskite fluoride, LixCoF3, with an exceptionally low tolerance factor has been synthesized through low-temperature lithium intercalation. The compound exhibits a high-temperature LiNbO3-type structure and undergoes a paramagnetic-to-antiferromagnetic transition.
A novel perovskite fluoride, LixCoF3, which has an exceptionally low tolerance factor (0.81), has been synthesized via low-temperature lithium intercalation into a distorted ReO3-type fluoride CoF3 using organolithium reagents. Interestingly, this reaction is completed within 15 min at room temperature. Synchrotron X-ray diffractometry and optical second harmonic generation at room temperature have revealed that this compound shows a high-temperature LiNbO3-type structure (space group: R (3$) over barc) involving Li-Co antisite defects and A-site splitting along the c direction. A-site splitting is consistent with the prediction based on hybrid Hartree-Fock density functional theory calculations. Co-L-2,L-3 edge X-ray absorption spectroscopy, as well as bond valence sum analysis, has verified the divalent oxidation state of Co ions in the lithiated phase, suggesting that its composition is close to LiCoF3 (x approximate to 1). This compound exhibits a paramagnetic-to-antiferromagnetic transition at 36 K on cooling, accompanied by weak ferromagnetic ordering. The synthetic route based on low-temperature lithiation of metal fluorides host paves the way for obtaining a new LiNbO3-type fluoride family.
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