The formation of
a protecting nanolayer, so-called solid electrolyte
interphase (SEI), on the negative electrode of Li-ion batteries (LIBs)
from product precipitation of the cathodic decomposition of the electrolyte
is a blessing since the electrically insulating nature of this nanolayer
protects the electrode surface, preventing continuous electrolyte
decomposition and enabling the large nominal cell voltage of LIBs,
e.g., 3.3–3.8 V. Thus, the protection performance of the nanolayer
SEI is essential for LIBs to achieve a long cycle life. Unfortunately,
the evaluation of this critical property of the SEI is not trivial.
Herein, a new, cheap, and easily implementable methodology, the redox-mediated
enhanced coulometry, is presented to estimate the protecting quality
of the SEI. The key element of the methodology is the addition of
a redox mediator in the electrolyte during the degassing step (after
the SEI formation cycle). The redox mediator leads to an internal
self-discharge process that is inversely proportional to the protecting
character of the SEI. Also, the self-discharge process results in
an easily measurable decrease in Coulombic efficiency. The influence
of vinylene carbonate as an electrolyte additive in the resulting
SEI is used as a case study to showcase the potential of the proposed
methodology.