Operando Identification of the Chemical and Structural Origin of Li-Ion Battery Aging at Near-Ambient Temperature

Min Seob Kim, Byoung Hoon Lee, Jae Hyuk Park, Hyeon Seok Lee, Wytse Hooch Antink, Euiyeon Jung, Jiheon Kim, Tae Yong Yoo, Chan Woo Lee, Chi Yeong Ahn, Seok Mun Kang, Jinsol Bok, Wonjae Ko, Xiao Wang, Sung Pyo Cho, Seung Ho Yu, Taeghwan Hyeon, Yung Eun Sung

Research output: Contribution to journalArticlepeer-review

26 Citations (Scopus)


Integrated with heat-generating devices, a Li-ion battery (LIB) often operates at 20-40 °C higher than the ordinary working temperature. Although macroscopic investigation of the thermal contribution has shown a significant reduction in the LIB performance, the molecular level structural and chemical origin of battery aging in a mild thermal environment has not been elucidated. On the basis of the combined experiments of the electrochemical measurements, Cs-corrected electron microscopy, and in situ analyses, we herein provide operando structural and chemical insights on how a mild thermal environment affects the overall battery performance using anatase TiO2 as a model intercalation compound. Interestingly, a mild thermal condition induces excess lithium intercalation even at near-ambient temperature (45 °C), which does not occur at the ordinary working temperature. The anomalous intercalation enables excess lithium storage in the first few cycles but exerts severe intracrystal stress, consequently cracking the crystal that leads to battery aging. Importantly, this mild thermal effect is accumulated upon cycling, resulting in irreversible capacity loss even after the thermal condition is removed. Battery aging at a high working temperature is universal in nearly all intercalation compounds, and therefore, it is significant to understand how the thermal condition contributes to battery aging for designing intercalation compounds for advanced battery electrode materials.

Original languageEnglish
Pages (from-to)13406-13414
Number of pages9
JournalJournal of the American Chemical Society
Issue number31
Publication statusPublished - 2020 Aug 5

Bibliographical note

Publisher Copyright:
Copyright © 2020 American Chemical Society.

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry
  • Biochemistry
  • Colloid and Surface Chemistry


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