Imparting Multi‐Scalar Architectural Control into Silk Materials Using a Simple Multi‐Functional Ice‐Templating Fabrication Platform

Human tissues and organs exhibit complex hierarchical gradient structures that are essential to their function should be recapitulated within biomaterial scaffolds targeting regeneration. Unidirectional freezing, an ice templating technique where acts as a porogen, is uniquely suited recapitulating the architectural anisotropy, gradients, transitions of human tissues, but polymeric systems, including silk fibroin, remains less well understood than colloidal counterparts. To address this, versatile accessible freezing setup for allows tuning parameters polymer cooling rate (30 °C min−1 2 min−1) solidification velocity (2.5 0.6 mm using liquid nitrogen, developed. Real time visual thermal monitoring process multiple concentrations (2–10% wt/v) material states (liquid, hydrogels) performed conditions correlated with pore morphology. Unprecedented control over size (100–90 000 µm2) morphology (cellular–lamellar), consistent alignment, generation porosity in demonstrated. For first time, impact shear thinning behavior crystal formation demonstrated, showing non-linear phenomena silk.