Graphene Oxide Precursor effects on 3D-Printed Carbon Scaffold

Abstract

Manganese oxide (MnO₂), an earth-abundant material, is a promising component for energy storage devices, having use in both pseudocapacitors and batteries. However, high MnO₂ loading often leads to reduced performance due to poor ion diffusion. 3D printing, particularly using the direct ink writing (DIW) technique, offers a solution by enabling the fabrication of electrodes with hierarchical porous structures and open channels that enhance mass transport and ion diffusion. Previous work demonstrated that 3D-printed graphene aerogels with MnO₂ coatings maintained excellent electrochemical performance, even with thick electrodes, due to their optimized structure. Building on this work, the current study investigates the performance differences between aerogels developed using graphene oxide (GO) and reduced graphene oxide (rGO) as carbon precursors. Both materials were incorporated into thixotropic inks, 3D-printed into lattice structures, and carbonized. Despite expected similarities between the final graphene aerogel, rGO-based aerogels exhibited superior areal capacitance, compared to GO-based aerogels. These differences are attributed to the lower oxygen content, and defect density of rGO, which influence its interaction with cellulose viscosifiers in the ink formulation. Brunauer-Emmett-Teller (BET) surface area analysis revealed that rGO aerogels possess a larger surface area and mesoporous structure, further enhancing their performance. When coated with MnO₂, rGO-based aerogels maintained their superior capacitive behavior over GO-based aerogels. This study highlights the effect of carbon precursor on the end performance of graphene aerogels.