The graphene oxide (GO) microstructure, in terms of flake distribution, folding, and crumpling, in thin films affects properties such as electrical conductivity and optical transparency after GO reduction. A thin film can be tailored to the user's application if the microstructure resulting from different deposition methods can be controlled. In this work, we compare the microstructures of GO coatings created through electrospray deposition (ESD) with random deposition processes. The comparisons include both MATLAB simulations and a dip coating process. The microstructure of ESD GO thin films can be altered by changing the distance between the nozzle and the substrate. We developed a semi-automatic image analysis script that analyzes scanning electron microscopy images to find effects of GO stacking or agglomeration, without the risk of human bias. A low nozzle to substrate distance creates structures of flat GO flakes, but solvent flooding the samples causes drying patterns. A high nozzle to substrate distance causes folding and crumpling of the GO flakes due to solvent evaporation, resulting in agglomerated GO on the substrate. For our ESD setup, a nozzle to substrate distance of 2-4 mm produced GO coatings with the lowest combined influence of drying effects and GO flake folding or crumpling.
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