Paper Title
OPTIMIZING BINDER-FREE ELECTROACTIVE INTERFACES BY CORRELATING DEPOSITION KINETICS AND MORPHOLOGY

Abstract
Binder-free organic electrodes are promising for next-generation batteries due to their elimination of inactive components and reduced interfacial resistance. However, their performance is often hindered by poor control over deposition kinetics and ion transport pathways. This study reveals a direct link between nucleation dynamics, morphology, and electrochemical transport in pyrene-derived interfaces created via intramolecular electrochemical oxidative cyclodehydrogenation (i-EoC), using techniques like cyclic voltammetry and pulse reverse electrodeposition (PRE). Unlike conventional methods that produce either compact films or dense layers with limited ionic mobility, PRE allows for dynamic interfacial reorganization and controlled nucleation, resulting in porous oligopyrene networks anchored to the current collector. The optimal PRE condition (pPy 90) balances electrochemically active surface area (0.45 cm²) and ion diffusion (2.01 x 10⁻⁶ cm²/s), lowers charge-transfer resistance, and ensures stability throughout extended cycling. This demonstrates that performance improvements stem from optimization of morphology and transport rather than higher molecular weight, establishing PRE as a scalable method to design binder-free organic battery electrodes for sodium-ion batteries with enhanced architectural efficiency. Keywords - Pulse reverse electrodeposition, Oligopyrene films, Intramolecular electrochemical oxidative cyclodehydrogenation, Ion transport, Deposition kinetics–morphology relationship, Binder-free electrodes.