title: Probing the degradation mechanisms in electrolyte solutions for Li-ion batteries by in situ transmission electron microscopy.
abstract: Development of novel electrolytes with increased electrochemical stability is critical for the next generation battery technologies. In situ electrochemical fluid cells provide the ability to rapidly and directly characterize electrode/electrolyte interfacial reactions under conditions directly relevant to the operation of practical batteries. In this paper, we have studied the breakdown of a range of inorganic/salt complexes relevant to state-of-the-art Li-ion battery systems by in situ (scanning) transmission electron microscopy ((S)TEM). In these experiments, the electron beam itself caused the localized electrochemical reaction that allowed us to observe electrolyte breakdown in real-time. The results of the in situ (S)TEM experiments matches with previous stability tests performed during battery operation and the breakdown products and mechanisms are also consistent with known mechanisms. This analysis indicates that in situ liquid stage (S)TEM observations could be used to directly test new electrolyte designs and identify a smaller library of candidate solutions deserving of more detailed characterization. A systematic study of electrolyte degradation is also a necessary first step for any future controlled in operando liquid (S)TEM experiments intent on visualizing working batteries at the nanoscale.
authors.affiliation: Fundamental and Computational Sciences Directorate and ‡Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352, United States.
authors.forename: Patricia
authors.initials: P
authors.lastname: Abellan
authors.forename: B Layla
authors.initials: BL
authors.lastname: Mehdi
authors.forename: Lucas R
authors.initials: LR
authors.lastname: Parent
authors.forename: Meng
authors.initials: M
authors.lastname: Gu
authors.forename: Chiwoo
authors.initials: C
authors.lastname: Park
authors.forename: Wu
authors.initials: W
authors.lastname: Xu
authors.forename: Yaohui
authors.initials: Y
authors.lastname: Zhang
authors.forename: Ilke
authors.initials: I
authors.lastname: Arslan
authors.forename: Ji-Guang
authors.initials: JG
authors.lastname: Zhang
authors.forename: Chong-Min
authors.initials: CM
authors.lastname: Wang
authors.forename: James E
authors.initials: JE
authors.lastname: Evans
authors.forename: Nigel D
authors.initials: ND
authors.lastname: Browning