Insights into the Solubility of Poly(vinylphenothiazine) in Carbonate-Based Battery Electrolytes

Autor: Verena Küpers, Peter Bieker, Martin Winter, Birgit Esser, Verena Perner, Fabian Otteny, Diddo Diddens, Martin Kolek
Rok vydání: 2021
Předmět:
Zdroj: ACS applied materials & interfaces 13(10), 12442-12453 (2021). doi:10.1021/acsami.0c20012
ISSN: 1944-8252
Popis: Organic materials are promising candidates for next-generation battery systems. However, many organic battery materials suffer from high solubility in common battery electrolytes. Such solubility can be overcome by introducing tailored high-molecular-weight polymer structures, for example, by cross-linking, requiring enhanced synthetic efforts. We herein propose a different strategy by optimizing the battery electrolyte to obtain insolubility of non-cross-linked poly(3-vinyl-N-methylphenothiazine) (PVMPT). Successive investigation and theoretical insights into carbonate-based electrolytes and their interplay with PVMPT led to a strong decrease in the solubility of the redox polymer in ethylene carbonate/ethyl methyl carbonate (3:7) with 1 M LiPF6. This allowed accessing its full theoretical specific capacity by changing the charge/discharge mechanism compared to previous reports. Through electrochemical, spectroscopic, and theoretical investigations, we show that changing the constituents of the electrolyte significantly influences the interactions between the electrolyte molecules and the redox polymer PVMPT. Our study demonstrates that choosing the ideal electrolyte composition without chemical modification of the active material is a successful strategy to enhance the performance of organic polymer-based batteries.
Databáze: OpenAIRE