Bridging papermaking and hydrogel production: Nanoparticle-loaded cellulosic hollow fibers with pitted walls as skeleton materials for multifunctional electromagnetic hydrogels

Electromagnetic hydrogels have attracted significant attention due to their vast potential in soft robotics, biomedical engineering, and energy harvesting. To facilitate future commercialization via large-scale industrial processes, we present a facile concept that utilizes the specialized knowledge of papermaking to fabricate hydrogels with multifunctional electromagnetic properties. The principles of papermaking wet end chemistry, which involves the handling of interactions among cellulosic fibers, fines, polymeric additives, and other components in aqueous systems, serves as a key foundation for this concept. Notably, based on these principles, the versatile use of chemical additives in combination with cellulosic materials enables the tailored design of various products. Our methodology exploits the unique hierarchically pitted and hollow tube-like structures of papermaking grade cellulosic fibers with discernible pits, enabling the incorporation of magnetite nanoparticles through lumen loading. By combining microscale softwood-derived cellulosic fibers with additives, we achieve dynamic covalent interactions that transform the cellulosic fiber slurry into an impressive hydrogel. The cellulosic fibers act as a skeleton, providing structural support within the hydrogel framework and facilitating the dispersion of nanoparticles. In accordance with our concept, the typical hydrogel exhibits combined attributes, including electrical conductivity, self-healing properties, pH responsiveness, and dynamic rheologic behavior. Our approach not only yields hydrogels with interesting properties but also aligns with the forefront of advanced cellulosic material applications. These materials hold the promise in remote strain sensing devices, electromagnetic navigation systems, contactless toys, and flexible electronic devices. The concept and findings of the current work may shed light on materials innovation based on traditional pulp and paper processes. Furthermore, the facile processes involved in hydrogel formation can serve as valuable tools for chemistry and materials education, providing easy demonstrations of principles for university students at different levels.