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      Operando investigations of the interfacial electrochemical kinetics of metallic lithium anodes via temperature-dependent electrochemical impedance spectroscopy

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      Embargo Lift Date: 2023-06-28
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      Author(s)
      Zabara, Mohammed Ahmed
      Katırcı, Gökberk
      Ülgüt, Burak
      Date
      2022-06-28
      Source Title
      Journal of Physical Chemistry C
      Print ISSN
      0002-7863
      Electronic ISSN
      1520-5126
      Publisher
      American Chemical Society
      Volume
      126
      Issue
      27
      Pages
      10968 - 10976
      Language
      English
      Type
      Article
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      Abstract
      One of the major hurdles in the utilization of metallic lithium anodes is understanding the Li+transfer kinetics through the solid electrolyte interface (SEI) in addition to Li oxidation. Electrochemical impedance spectroscopy (EIS) combined with temperature variation provides deeper comprehension and reveals kinetic parameters of individual processes separately. In this study, we report temperature-dependent EIS analysis of metallic Li anodes to shed light on the kinetics of anodic/interfacial processes at different states of charge and wide temperature ranges (-25 to 75 °C), utilizing lithium thionyl chloride (Li/SOCl2) and lithium manganese dioxide (Li/MnO2) primary batteries as model systems. We found in both batteries that the impedance of the SEI processes is highly temperature-dependent with non-Arrhenius behavior at temperatures greater than 35 °C. Conversely, the kinetics of the anodic process showed small temperature dependence that is explained by the Arrhenius equation throughout the temperature range studied. The results provide a deeper understanding of the underlying processes separately in metallic Li anodes under operando and real-time conditions. © 2022 American Chemical Society. All rights reserved.
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      http://hdl.handle.net/11693/111640
      Published Version (Please cite this version)
      https://dx.doi.org/10.1021/acs.jpcc.2c02396
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