Universal Solvent Escape Strategies for Efficient Curing of Hydrogen-Bond-Rich 3D Printing Inks

Hydrogen-bonded polymers have attracted significant interest in biomedical applications due to their excellent biocompatibility, adjustable mechanical properties, and responsiveness to environmental cues. However, these materials face substantial challenges in direct ink writing, primarily arising from persistent solvent entrapment within dense hydrogen-bonded networks. This trapped solvent severely impairs the printability, drying efficiency, and structural fidelity of scaffolds. To overcome these limitations, this study introduced innovative universal solvent escape strategies integrating three key mechanisms: first, solvent replacement disrupted existing hydrogen-bonded polymer complexes; second, nanoparticle-induced microturbulence significantly enhanced solvent evaporation rates; third, computationally optimized printing paths facilitated efficient solvent evacuation. Molecular dynamics simulations provided quantitative insights into how various ways can effectively destroy hydrogen bond solvent networks, allowing rapid solvent removal. Finite element analysis accurately visualized the curing behavior to maximize solvent extraction. This integrated strategy enabled exceptionally rapid (< 3 min) and structurally precise scaffold fabrication across diverse hydrogen-bonded polymers, including chitosan, collagen, and cellulose. Furthermore, these scaffolds exhibited multifunctional capabilities, utilizing hydrogen-bonding networks for both structural integrity and pH-responsive drug delivery. Functional scaffold confirmed significantly improved osteogenic and angiogenic performance via enhanced calcium signaling and activation of HIF-1α pathways, thereby advancing the fields of tissue engineering and controlled therapeutic delivery.