Journal
CHEMPHYSCHEM
Volume 16, Issue 6, Pages 1179-1189Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cphc.201402674
Keywords
overcharge protection; phenothiazine; radical cations; redox shuttles; substituent effects
Funding
- University of Kentucky's Office for the Vice President for Research
- University of Kentucky's College of Arts and Sciences
- American Chemical Petroleum Research Fund
- National Science Foundation, Division of Chemistry [CHE-1300653]
- Direct For Mathematical & Physical Scien [1300653] Funding Source: National Science Foundation
- Division Of Chemistry [1300653] Funding Source: National Science Foundation
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Phenothiazine and five N-substituted derivatives were evaluated as electrolyte additives for overcharge protection in LiFePO4/synthetic graphite lithium-ion batteries. We report on the stability and reactivity of both the neutral and radical-cation forms of these six compounds. While three of the compounds show extensive overcharge protection, the remaining three last for only one to a few cycles. UV/Vis studies of redox shuttle stability in the radical cation form are consistent with the overcharge performance: redox shuttles with spectra that show little change over time exhibit extensive overcharge performance, whereas those with changing spectra have limited overcharge protection. In one case, we determined that a CN bond cleaves upon oxidation, forming the phenothiazine radical cation and leading to premature overcharge protection failure; in another case, poor solubility appears to limit protection.
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