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Operando fluorescence lifetime imaging microscopy during Li+ intercalation into graphitic electrodes.
Matthew J Quarrell1, Thukshan Samarakoon1, Alex R Neale1
1Stephenson Institute for Renewable Energy, Department of Chemistry, University of Liverpool, Liverpool, L69 7ZD, UK. hardwick@liverpool.ac.uk.
Summary
Operando fluorescence lifetime imaging microscopy revealed distinct emission backgrounds in lithium-ion cells. Differences in graphite electrode emission during cycling were linked to electrolyte salt stability, specifically comparing lithium hexafluorophosphate and lithium perchlorate.
Area of Science:
- Electrochemistry
- Materials Science
- Spectroscopy
Background:
- Understanding electrolyte degradation is crucial for lithium-ion battery longevity.
- Emission background evolution in lithium-ion cells impacts performance monitoring.
- Salt stability significantly influences electrolyte behavior during battery cycling.
Purpose of the Study:
- To investigate the evolution of emission background in lithium-ion half-cells.
- To spatially map fluorescence lifetimes on graphite electrodes during electrochemical cycling.
- To compare the impact of different electrolyte salt formulations on emission characteristics.
Main Methods:
- Utilized operando fluorescence lifetime imaging microscopy.
- Performed spatial mapping of fluorescence lifetimes on graphite electrodes.
- Analyzed lithiation and delithiation processes in two distinct electrolyte formulations.
Main Results:
- Observed differing emission characteristics associated with electrolyte salt stability.
- Highlighted variations in fluorescence lifetimes on graphite electrodes.
- Demonstrated a correlation between salt type (Li[PF6] vs. Li[ClO4]) and emission background evolution.
Conclusions:
- Electrolyte salt stability plays a key role in the observed emission background changes.
- Fluorescence lifetime imaging microscopy is a valuable tool for probing electrode-electrolyte interfaces.
- The study provides insights into degradation mechanisms influenced by electrolyte composition.

