Solution Property Windows Governing Electrospinning of Natural Polymers in Acetic Acid

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ABSTRACT Understanding the coupling between rheological behavior, interfacial properties and electrohydrodynamic stability is essential for engineering electrospinnable polymer systems. However, a unified and comparative understanding across different classes of biopolymers remains limited, particularly under consistent solvent and processing conditions. In this study, chitosan, gelatin, zein, and cellulose acetate dissolved in acetic acid are electrospun under comparable conditions to elucidate the effects of conductivity, viscosity, and surface tension on fiber formation as a function of concentration. Continuous fiber formation is achieved within a viscosity window of 0.3 to 6.0 Pa·s and a surface tension range of 24 to 26 mN m −1 . This experimentally identified processing window is in strong agreement with predictions based on the Ohnesorge number, confirming that sufficient polymer chain entanglement must overcome surface tension forces to suppress capillary breakup and enable stable jet formation. The resulting fiber morphology is governed by a coupled interplay between dispersion properties, where viscosity controls jet stability and fiber diameter, surface tension defines the spinnability threshold, and conductivity provides a secondary contribution through electrostatic stretching. Furthermore, opposing wettability trends were observed between polymer classes: increasing fiber diameter led to enhanced hydrophobicity in carbohydrate‐based systems, whereas protein‐based fibers exhibited increased hydrophilicity, highlighting the dominant role of surface chemistry over morphology. Overall, this study establishes empirical thresholds for the efficient electrospinning of natural polymers and introduces a sustainable concentration‐regulated method to modulate fiber wettability without chemical modification. These findings provide a scalable and sustainable framework for designing functional, non‐toxic biopolymer mats for applications spanning food and therapeutic systems, biomedical engineering, filtration membranes, packaging, wearable materials, and electronics.

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