Electrolyte Oxidation Pathways in Lithium-Ion Batteries

Journal of the American Chemical Society
Bernardine L. D. RinkelClare P. Grey

Abstract

The mitigation of decomposition reactions of lithium-ion battery electrolyte solutions is of critical importance in controlling device lifetime and performance. However, due to the complexity of the system, exacerbated by the diverse set of electrolyte compositions, electrode materials, and operating parameters, a clear understanding of the key chemical mechanisms remains elusive. In this work, operando pressure measurements, solution NMR, and electrochemical methods were combined to study electrolyte oxidation and reduction at multiple cell voltages. Two-compartment LiCoO2/Li cells were cycled with a lithium-ion conducting glass-ceramic separator so that the species formed at each electrode could be identified separately and further reactions of these species at the opposite electrode prevented. One principal finding is that chemical oxidation (with an onset voltage of ∼4.7 V vs Li/Li+ for LiCoO2), rather than electrochemical reaction, is the dominant decomposition process at the positive electrode surface in this system. This is ascribed to the well-known release of reactive oxygen at higher states-of-charge, indicating that reactions of the electrolyte at the positive electrode are intrinsically linked to surface reactivity ...Continue Reading

References

May 11, 2006·Environmental Science & Technology·William F FinneyLarry W Beck
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Oct 7, 2016·Physical Chemistry Chemical Physics : PCCP·S Wiemers-MeyerS Nowak
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Citations

Dec 10, 2020·Nature Communications·Clare P Grey, David S Hall
Aug 7, 2021·Scientific Data·Evan Walter Clark Spotte-SmithKristin Aslaug Persson
Aug 12, 2021·Journal of the American Chemical Society·Xiaowei XieKristin A Persson
Sep 4, 2021·The Journal of Physical Chemistry. C, Nanomaterials and Interfaces·Svetlana MenkinClare P Grey
Sep 15, 2021·Angewandte Chemie·Darren M C OuldDominic S Wright

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