Network architecture dependent mechanical response in temperature responsive collagen-PNIPAM composites

Collagen is the most abundant protein in the mammalian extracellular matrix. In-vitro collagen-based materials with specific mechanical properties are important for various bio-medical and tissue-engineering applications. Here, we study the reversible mechanical switching behaviour of a bio-compatible composite formed by collagen networks seeded with thermo-responsive poly(N-isopropylacrylamide) (PNIPAM) microgel particles, by exploiting the swelling/de-swelling of the particles across the lower critical solution temperature (LCST). Interestingly, we find that the shear modulus of the system reversibly enhances whenever the diameter of the microgel particles is changed from that corresponding to the polymerization temperature of the composite, irrespective of swelling or, de-swelling. However, the degree of such enhancement significantly depends on the temperature-dependent collagen network architecture quantified by the mesh size of the network. Furthermore, confocal imaging of the composite during the temperature switching reveals that the reversible clustering of microgel particles above LCST plays a crucial role in the observed switching response.