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Cited by 455

The DOI matches its Crossref record; 66 of the 66 references it cites were found in a registry or an index.

Electrolyte Oxidation Pathways in Lithium-Ion Batteries

Open access
Rinkel, Bernardine L. D., Hall, David S., Temprano, Israel, Grey, Clare P.·2020·Journal of the American Chemical Society
DOI 10.1021/jacs.0c06363
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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 LiCoO 2 /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 LiCoO 2 ), 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 of the active material. Soluble electrolyte decomposition products formed at both electrodes are characterised, and a detailed reaction scheme is constructed to rationalise the formation of the observed species. The insights on electrolyte decomposition through reactions with reactive oxygen species identified through this work have direct impact on understanding and mitigating degradation in high voltage/higher energy density LiCoO 2 -based cells, and more generally for cells containing nickel-containing cathode materials (e.g. LiNi x Mn y Co z O 2 ; NMCs), as they lose oxygen at lower operating voltages.

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Metadata

Authors
Rinkel, B. L. D., Hall, D. S., Temprano, I., & Grey, C. P.
Venue
Journal of the American Chemical Society
Publisher
American Chemical Society (ACS)
Published
2020-07-22
Volume
142
Issue
35
Pages
15058-15074
ISSN
  • 0002-7863 (ISSN-L)
  • 1520-5126
DOI
10.1021/jacs.0c06363
OpenAlex
W3044365402
Cited by
455
References
66
FWCI
13.08
Type
journal article
Language
en
Open access
green

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