Simultaneous One‐Pot Interpenetrating Network Formation to Expand 3D Processing Capabilities. Issue 28 (4th June 2022)

• Record Type: Journal Article
• Authors: Dhand, Abhishek P.; Davidson, Matthew D.; Galarraga, Jonathan H.; Qazi, Taimoor H.; Locke, Ryan C.; Mauck, Robert L.; Burdick, Jason A.
• Is Part Of: Advanced materials. Volume 34:Issue 28(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-06-04
• Subjects: Digital Light Processing -- hydrogels -- interpenetrating polymer networks -- microparticles -- photo‐crosslinking; Materials -- Periodicals; Chemical vapor deposition -- Periodicals; 620.11
• DOI: 10.1002/adma.202202261
• Languages: English
• ISSNs: 0935-9648

Abstract

Abstract: The incorporation of a secondary network into traditional single‐network hydrogels can enhance mechanical properties, such as toughness and loading to failure. These features are important for many applications, including as biomedical materials; however, the processing of interpenetrating polymer network (IPN) hydrogels is often limited by their multistep fabrication procedures. Here, a one‐pot scheme for the synthesis of biopolymer IPN hydrogels mediated by the simultaneous crosslinking of two independent networks with light, namely: i) free‐radical crosslinking of methacrylate‐modified hyaluronic acid (HA) to form the primary network and ii) thiol–ene crosslinking of norbornene‐modified HA with thiolated guest–host assemblies of adamantane and β‐cyclodextrin to form the secondary network, is reported. The mechanical properties of the IPN hydrogels are tuned by changing the network composition, with high water content (≈94%) hydrogels exhibiting excellent work of fracture, tensile strength, and low hysteresis. As proof‐of‐concept, the IPN hydrogels are implemented as low‐viscosity Digital Light Processing resins to fabricate complex structures that recover shape upon loading, as well as in microfluidic devices to form deformable microparticles. Further, the IPNs are cytocompatible with cell adhesion dependent on the inclusion of adhesive peptides. Overall, the enhanced processing of these IPN hydrogels will expand their utility across applications. Abstract : A one‐pot photoinitiated reaction strategy is utilized to create tough interpenetrating polymer network (IPN) hydrogels that are amenable to processing modalities such as Digital Light Processing based 3D printing and microfluidic fabrication of microparticles. The mechanical properties of these IPN hydrogels are highly tunable with optimal formulations exhibiting high toughness and low hysteresis despite the high water content.