Journal
JOURNAL OF POWER SOURCES
Volume 509, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.jpowsour.2021.230376
Keywords
Electrochemical impedance; All-solid-state battery; Lithium ion; Charge transfer resistance; Degradation mechanism; Oxidation
Funding
- project of Development of Fundamental Technologies for All Solid State Battery applied to Electric Vehicles(SOLiD-EV) [JPNP18003]
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The research highlights the importance of the active material coating of a cathode in all-solid-state lithium-ion batteries for charge transfer. The study also shows that cathodes with a LiNbO3 coating exhibit different charge transfer resistance trends after durability tests at various charging potentials. In addition, oxidation of sulfide at the solid electrolyte-coating interface was observed using time-of-flight secondary-ion mass spectrometry.
The active material coating of a cathode in all-solid-state lithium-ion batteries using sulfide-based solid electrolytes is known to be an essential technology. Electrochemical impedance spectroscopic measurements showed that two charge-transfer processes occurred at the interface between an argyrodite-type sulfide solid electrolyte and LiNi0.5Co0.2Mn0.3O2 both with and without a LiNbO3 coating. The process in the higher-frequency region was attributed to the solid electrolyte-coating and/or the coating itself, whereas that in the lower-frequency region was attributed to the lithiation/delithiation of the cathode active material. The two charge transfer resistances observed in the cell with a LiNbO3-coated cathode-after durability tests at various charging potentials-exhibited different trends. The charge transfer resistance was maintained at 4.55 V vs. Li/Li+, and only one at the higher frequency increased. The oxidation of sulfide at the solid electrolyte-coating interface was observed using time-of-flight secondary-ion mass spectrometry. However, the degradation at the active material surface was not observed using transmission electron microscope/electron energy loss spectroscopy. The results of the material analyses support the ascription of impedance spectra and their associated resistance trends in the durability test.
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