Abstract
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.
Highlights
With every year’s growing demand of systems for energy supply, new approaches for the storage of renewable energies are required
Actions between PVMPT and the individual components of the electrolyte mixtures based on molecular dynamics (MD) simulation data and present a solution to reduce the solubility of the non-cross-linked redox polymer by the correct choice of Cyclic voltammetry (CV) measurements were conducted on a VMP3 potentiostat (BioLogic Science Instruments) using 500 μV s−1
General battery understanding suggests that the solubility of the active material in the battery electrolyte results in battery cell deterioration (“aging”) indicated by severe capacity losses.[49,50]
Summary
With every year’s growing demand of systems for energy supply, new approaches for the storage of renewable energies are required. The polymer was cross-linked in X-PVMPT, the solubility in the electrolyte was reduced, and the lost capacity could be regained but at the cost of rate capability.[26] blends were prepared in a nitrogen atmosphere (glove box) using 1 M (mol L−1) conducting salt in EC/DMC (1:1 by wt), EC/DMC (3:7 by wt), EC/EMC (1:1 by wt), or EC/EMC (3:7 by wt). We follow another approach to control the solubility chemical measurements were performed in a three-electrode setup of PVMPT during battery cycling. Actions between PVMPT and the individual components of the electrolyte mixtures based on molecular dynamics (MD) simulation data and present a solution to reduce the solubility of the non-cross-linked redox polymer by the correct choice of Cyclic voltammetry (CV) measurements were conducted on a VMP3 potentiostat (BioLogic Science Instruments) using 500 μV s−1. Shorter simulation runs of the carbonate electrolytes were performed for force field validation (see the Supporting Information for further details)
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