This study explored the influence of graphene oxide (GO) on morphological and mechanical properties of Nafion^® 115 membranes with the objective of enhancing the mechanical properties of the most widely employed membrane in Proton Exchange Membrane Water Electrolyzers (PEMWE) applications. The membrane surface was modified by ultrasonically spraying a GO solution and different annealing temperatures were tested. Scanning Electron Microscopy (SEM) cross-sectional images revealed that annealing the composite membranes was sufficient to favor an interaction between the graphene oxide and the surface of the Nafion^® membranes. The GO covering only 35% of the membrane surface increased the composite’s wettability from hydrophobic (105.2°) to a highly hydrophilic angle (84.4°) while slightly reducing membrane swelling. Tensile tests depicted an increase in both the strain levels and tensile loads before breaking. The samples with GO presented remarkable mechanical properties when the annealing time and temperature increased; while the Nafion^® control samples failed at elongations of 95% and 98%, their counterparts with GO on the surface achieved elongations of 248% and 191% when annealed at 80 °C and 110 °C respectively, demonstrating that the presence of GO mechanically stabilizes the membranes under tension. In exchange, the presence of GO altered the smoothness of the membrane surface going from an average 1.4 nm before the printing to values ranging from 8.4 to 10.2 nm depending on the annealing conditions which could affect the quality of the subsequent catalyst layer printing. Overall, the polymer’s electrical insulation was unaffected, making the Nafion^®-GO blend a more robust material than those traditionally used.

The PDI-EH molecule was synthesized and integrated into ternary OSCs to obtain miscibility-driven morphology optimization. The relationship between the optimized morphology and charge carrier dynamics was explored by PiFM and TP-AFM characterization.