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Operando Optical Imaging of Cathode Swelling Process Inside Lithium Primary Batteries: Comparative Studies between

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Summary

Fluorinated carbon (CF) cathodes show promise for lithium batteries but swell during discharge. Hard carbon-derived CF (FHC) exhibits less swelling than fluorinated graphite (FG) due to more uniform lithium insertion.

Keywords:
electrochemical lithiationfluorinated carbonlithium primary batteryoperando optical imagingsingle-particle spectroscopy

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Fluorinated carbon (CF) is a high-capacity cathode material for lithium primary batteries.
  • Nonuniform volume expansion during discharge limits the performance of CF cathodes.
  • Understanding CF swelling mechanisms is crucial for optimizing battery performance.

Purpose of the Study:

  • To investigate the volume evolution of different CF cathode structures during discharge.
  • To quantify swelling ratios and correlate them with electrochemical lithiation mechanisms.
  • To elucidate the factors influencing cathode swelling in Li/CF batteries.

Main Methods:

  • Operando confocal microscopy was employed to visualize cathode thickness changes.
  • Swelling ratios were quantified as a function of discharge depth.
  • Single-particle Raman and photoluminescence spectroscopy were used to study lithiation mechanisms.

Main Results:

  • Hard carbon-derived fluorinated carbon (FHC) showed a lower swelling ratio compared to fluorinated graphite (FG).
  • FHC, with its disordered structure and pores, exhibited more homogeneous lithiation.
  • FG displayed nonuniform lithium insertion via 'edge propagation' pathways, leading to greater swelling.

Conclusions:

  • The study reveals distinct electrochemical mechanisms governing volume expansion in different CF structures.
  • Homogeneous lithiation in FHC effectively mitigates cathode swelling.
  • Findings provide insights for designing advanced CF cathodes with improved electrochemical stability and performance in Li/CF batteries.