Exploring the Synergistic Effects of Inactive Materials and Processing on Aqueous Fabrication of Poly(3‐Vinyl‐ N ‐Methylphenothiazine) Positive Electrodes for Lithium‐Organic Batteries

Organic redox-active electrode materials are gaining increasing attention due to their eco-friendliness, abundance, and structural versatility. However, their processing typically depends on poly(vinylidene difluoride) (PVdF) as binder and N-methyl-2-pyrrolidone (NMP) as solvent, both are expensive and hazardous. While aqueous processing methods are well established for inorganic electrodes, their application to organic materials remains largely unexplored. This study investigates the use of water-processable binders, specifically sodium carboxymethyl cellulose (Na-CMC) and styrene-butadiene rubber (SBR) for fabricating poly(3-vinyl-N-methylphenothiazine) electrodes. Key factors influencing electrode performance and microstructure were systematically studied, including the choice of conductive additive, mixing procedures, hot-pressing, and densification. Among these, the selection of conductive additive, mixing method, and room temperature densification at different pressure had the most pronounced impact on electrochemical performance. Electrodes using Na-CMC as the primary binder retained ≈90% of their theoretical capacity over 1000 cycles at 1C rate, comparable to PVdF-based electrodes. While increased densification pressure improved electrode uniformity, it had a detrimental effect on electrochemical performance. Introducing SBR as a co-binder at various weight ratios enhanced mechanical integrity and mitigated the negative effects of high densification pressure, ultimately leading to improved electrochemical performance under these applied operation conditions.