Poly(Ethylene Oxide)-based Electrolyte for Solid-State-Lithium-Batteries with High Voltage Positive Electrodes: Evaluating the Role of Electrolyte Oxidation in Rapid Cell Failure.

Scientific Reports
Gerrit HomannJohannes Kasnatscheew

Abstract

Polyethylene oxide (PEO)-based solid polymer electrolytes (SPEs) typically reveal a sudden failure in Li metal cells particularly with high energy density/voltage positive electrodes, e.g. LiNi0.6Mn0.2Co0.2O2 (NMC622), which is visible in an arbitrary, time - and voltage independent, "voltage noise" during charge. A relation with SPE oxidation was evaluated, for validity reasons on different active materials in potentiodynamic and galvanostatic experiments. The results indicate an exponential current increase and a potential plateau at 4.6 V vs. Li|Li+, respectively, demonstrating that the main oxidation onset of the SPE is above the used working potential of NMC622 being < 4.3 V vs. Li|Li+. Obviously, the SPE│NMC622 interface is unlikely to be the primary source of the observed sudden failure indicated by the "voltage noise". Instead, our experiments indicate that the Li | SPE interface, and in particular, Li dendrite formation and penetration through the SPE membrane is the main source. This could be simply proven by increasing the SPE membrane thickness or by exchanging the Li metal negative electrode by graphite, which both revealed "voltage noise"-free operation. The effect of membrane thickness is also valid with LiFePO4 ...Continue Reading

References

Nov 20, 2001·Nature·J M Tarascon, M Armand
Mar 5, 2015·Physical Chemistry Chemical Physics : PCCP·Georg BiekerPeter Bieker
Jun 10, 2015·ACS Applied Materials & Interfaces·Lorenzo CarboneJusef Hassoun
Jan 16, 2016·Physical Chemistry Chemical Physics : PCCP·J KasnatscheewM Winter
Mar 17, 2017·Topics in Current Chemistry·Isidora Cekic-LaskovicMartin Winter
Sep 20, 2017·Physical Chemistry Chemical Physics : PCCP·Florian HoltstiegeTobias Placke
Apr 20, 2018·Topics in Current Chemistry·Johannes KasnatscheewIsidora Cekic-Laskovic
Dec 1, 2018·Chemical Reviews·Martin WinterKang Xu

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