Thermal and Structural Properties of Amphiphilic Polyelectrolyte Complexes

Amphiphilic polyelectrolytes (APEs) offer significant promise for advanced applications, particularly as fouling‐resistant filtration membranes. This work reports a detailed investigation of APEs focused on their thermophysical properties, structural characteristics, surface wettability, and, for the first time, their electrospinnability. The APEs are formed from cationic poly(methyl methacrylate‐ co ‐[2(methacryloyloxy)ethyl] trimethylammonium chloride), referred to as C+, and anionic poly(methyl methacrylate‐ co ‐2‐sulfoethyl methacrylate), referred to as C−. Thermal analysis revealed glass transition temperatures, T g , of 112°C for C− and 156°C for C+. C+ and C− were blended at different compositions to vary the relative proportions of positive and negative units. T g increased as the C+ content increased. The heat capacity increment at T g , Δ c p ( T g ), of the blends was analyzed using the Wunderlich bead model to characterize the level of molecular confinement. Δc p ( T g ) generally increased as C+ content increased, leading to a reduction in confinement. These results demonstrate that the thermal properties of the blends can be tuned through compositional variation. The C+/C− blends exhibit hydrophilic surfaces with water contact angles ranging from 60°–71°. C+/C− blends were successfully electrospun to form micron‐scale nanofibers (diameters in the range of 0.43–5.10 μm). These findings provide a foundational thermophysical and processing dataset, demonstrating their potential for use in advanced separation technologies.