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Abstract Fused deposition modeling 3D printing provides a cost-effective and streamlined method for producing electrochemical sensors, overcoming the challenges associated with material selection, complex fabrication processes, and reproducibility issues. This study introduces an innovative approach utilizing a dual-printer setup to simplify the manufacturing of sensor electrodes. A critical enhancement in this process is the surface modification with reduced graphene oxide (rGO), which not only improves the electrochemical characteristics but also induces a wrinkled structure on the 3D printed surface. These wrinkles significantly increase the surface area, directly boosting the electrode’s electrochemical performance. Comprehensive characterization of the electrode surfaces, both before and after rGO modification, demonstrates a substantial increase in sensitivity, with a fortyfold improvement observed in hydrogen peroxide (H₂O₂) amperometric measurements. This breakthrough paves the way for advanced applications in 3D printed electrochemical sensors. 

Abstract Graphene-based electrodes have been extensively investigated for supercapacitor applications. However, their ion diffusion efficiency is often hindered by the graphene restacking phenomenon. Even though holey graphene is fabricated to address this issue by providing ion transport channels, those channels could still be blocked by densely stacked graphene nanosheets. To tackle this challenge, this research aims at improving the ion diffusion efficiency of microwave-synthesized holey graphene films by tuning the water interlayer spacer towards the improved supercapacitor performance. By controlling the vacuum filtration during graphene-based electrode fabrication, we obtain dry films with dense packing and wet films with sparse packing. The SEM images reveal that 20 times larger interlayer distance is constructed in the wet film compared to that in the dry counterpart. The holey graphene wet film delivers a specific capacitance of 239 F/g, ~82% enhancement over the dry film (131 F/g). By an integrated experimental and computational study, we quantitatively show that the interlayer spacing in combination with the nanoholes in the basal plane dominates the ion diffusion rate in holey graphene-based electrodes. Our study concludes that novel hierarchical structures should be further considered even in holey graphene thin films to fully exploit the superior advantages of graphene-based supercapacitors. 

Graphene with in-plane nanoholes, named holey graphene, shows great potential in electrochemical applications due to its fast mass transport and improved electrochemical activity. Scalable nanomanufacturing of holey graphene is generally based on chemical etching using hydrogen peroxide to form through-the-thickness nanoholes on the basal plane of graphene. In this study, we probe into the fundamental mechanisms of nanohole formation under peroxide etching via an integrated experimental and computational effort. The research results show that the growth of nanoholes during the etching of graphene oxide is achieved by a three-stage reduction–oxidation–reduction procedure. First, it is demonstrated that vacancy defects are formed via a partial reduction-based pretreatment. Second, hydrogen peroxide reacts preferentially with the edge-sites of defect areas on graphene oxide sheets, leading to the formation of various oxygen-containing functional groups. Third, the carbon atoms around the defects are removed along with the neighboring carbon atoms via reduction. By advancing the understanding of process mechanisms, we further demonstrate an improved nanomanufacturing strategy, in which graphene oxide with a high density of defects is introduced for peroxide etching, leading to enhanced nanohole formation.