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000874259 1001_ $$0P:(DE-Juel1)169878$$aHomann, Gerrit$$b0
000874259 245__ $$aPoly(Ethylene Oxide)-based Electrolyte for Solid-State-Lithium-Batteries with High Voltage Positive Electrodes: Evaluating the Role of Electrolyte Oxidation in Rapid Cell Failure
000874259 260__ $$a[London]$$bMacmillan Publishers Limited, part of Springer Nature$$c2020
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000874259 520__ $$aPolyethylene 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 electrodes. In summary, it is the cell set-up (PEO thickness, negative electrode), which is crucial for the voltage-noise associated failure, and counterintuitively not a high potential of the positive electrode.
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000874259 7001_ $$0P:(DE-Juel1)181055$$aStolz, Lukas$$b1
000874259 7001_ $$0P:(DE-Juel1)171863$$aNair, Jijeesh$$b2
000874259 7001_ $$0P:(DE-Juel1)171204$$aCekic-Laskovic, Isidora$$b3
000874259 7001_ $$0P:(DE-Juel1)166130$$aWinter, Martin$$b4
000874259 7001_ $$0P:(DE-Juel1)171865$$aKasnatscheew, Johannes$$b5$$eCorresponding author
000874259 773__ $$0PERI:(DE-600)2615211-3$$a10.1038/s41598-020-61373-9$$gVol. 10, no. 1, p. 4390$$n1$$p4390$$tScientific reports$$v10$$x2045-2322$$y2020
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