Bioderived Cyrene For Sustainably 3D Printing Organo/Hydrogels

Abstract

Hydrogels possess unique properties that make them suitable for a wide range of applications. Recent advances in 3D printing techniques, such as stereolithography (SLA), have enabled the precise customization of hydrogel structures with complex geometries and controlled mechanical properties. Further development of advanced hydrogel properties remains a key research focus, with particular attention to improving properties such as mechanical integrity, electrical conductivity, and responsiveness to environmental stimuli. Strategies such as incorporating fillers and nanofillers into hydrogel matrices have been explored to enhance these properties. Additionally, the use of organic solvents instead of water, leading to the formation of organogels, has begun to expand the range of printable materials, addressing some limitations associated with hydrogel-based SLA printing, such as structural disintegration. This thesis investigates the use of Cyrene, a bioderived and environmentally friendly solvent, as an alternative to traditional organic solvents in 3D-printed hydrogel systems. Organogels can be 3D printed, and afterwards a simple solvent exchange with water can convert organogels into the desired hydrogels materials, maintaining the advantage of biocompatibility along with the complex structures produced by SLA 3D printing. This research work started by exploring Cyrene’s role in hydrogel formulation, printability, and mechanical performance, comparing its effectiveness with the synthesis route using Cyrene and conventional solvents such as dimethyl sulfoxide (DMSO). Specifically, this study focuses on Cyrene’s application in mask stereolithography (mSLA) 3D printing of organogels. It demonstrates Cyrene’s excellent performance in enhancing hydrogel stretchability and swelling behavior after solvent exchange. Additionally, structural stability during organogel printing is improved due to the application of a previously developed acrylate salt. The findings reported in this work suggest that Cyrene-based hydrogels have promising applications in biomedical fields and soft robotics. Furthermore, we extend this investigation by examining Cyrene as a dispersion medium for graphene, and its use in hydrogel nanocomposites. The study highlights Cyrene’s ability to stabilize graphene dispersion without the need for chemical surfactants, aiming to produce hydrogels with enhanced mechanical strength, electrical conductivity, and multifunctional properties. These advancements open new investigations for applications in flexible electronics, biosensing, and tissue engineering. The research findings provide a comprehensive understanding of Cyrene’s potential as a sustainable solvent in the synthesis of organogels that can be converted into hydrogels after solvent exchange and used for a wide range of applications. The insights gained from this research contribute to the advancement of high-performance, eco-friendly hydrogel materials by demonstrating how Cyrene can serve as a sustainable alternative to conventional organic solvents. By utilizing a bioderived solvent to create organogels, followed by solvent exchange with water, the mechanical properties, structural stability, and biocompatibility of 3D-printed hydrogels can be enhanced. Additionally, the ability to stabilize graphene dispersion in hydrogels without chemical surfactants opens new opportunities for developing conductive and multifunctional hydrogel-based devices. These findings not only support the ongoing shift toward greener material synthesis but also lay the foundation for future innovations in sustainable material science and additive manufacturing.