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Atomic-scale observation of LiFePO4 and LiCoO2 dissolution behavior in aqueous solutions

Cited 24 time in Web of Science Cited 23 time in Scopus
Authors
Byeon, Pilgyu; Bae, Hyung Bin; Chung, Hee-Suk; Lee, Sang-Gil; Kim, Jin-Gyu; Lee, Hyeon Jeong; Choi, Jang Wook; Chung, Sung-Yoon
Issue Date
2018-11
Citation
Advanced Functional Materials, Vol.28 No.45, p. 1804564
Keywords
atomic-scale observationLi-intercalation oxidesSTEMstructure degradationsurface
Abstract
Understanding the atomic structure variation at the surface of electrode materials in contact with an electrolyte is an essential step toward achieving better electrochemical performance of rechargeable cells. Different types of water-based aqueous solutions are suggested as alternative electrolytes to the currently used flammable organic solvents in Li-ion batteries. However, most research on aqueous rechargeable Li-ion cells has largely focused on the synthetic processing of materials and resulting electrochemical properties rather than in-depth atomic-level observation on the electrode surface where the initial charge transfer and the (de)intercalation reaction take place. By using LiFePO4 and LiCoO2 single crystals, serious P and Co dissolution from LiFePO4 and LiCoO2 into aqueous solutions without any electrochemical cycling is identified. Furthermore, both strong temperature-dependent behavior of P dissolution in LiFePO4 and very unusual occupancy of Co in the tetrahedral interstices in LiCoO2 are directly demonstrated via atomic-scale (scanning) transmission electron microscopy. Ab initio density functional theory calculations also reveal that this tetrahedral-site occupation is stabilized when cation vacancies are simultaneously present in both Li and Co sites. The findings in this work emphasize the significance of direct observation on the atomic structure variation and local stability of the cathode materials.
ISSN
1616-301X
URI
https://hdl.handle.net/10371/164622
DOI
https://doi.org/10.1002/adfm.201804564
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College of Engineering/Engineering Practice School (공과대학/대학원)Dept. of Chemical and Biological Engineering (화학생물공학부)Journal Papers (저널논문_화학생물공학부)
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