Non-Linear Behaviour Of Gelatin Networks Reveals A Hierarchical Structure

We investigate the strain hardening behaviour of various gelatin networks - namely physically-crosslinked gelatin gel, chemically-crosslinked gelatin gels, and a hybrid gels made of a combination of the former two - under large shear deformations using the pre-stress, strain ramp, and large amplitude oscillation shear protocols. Further, the internal structures of physically-crosslinked gelatin gel and chemically-crosslinked gelatin gels were characterized by small angle neutron scattering (SANS) to enable their internal structures to be correlated with their nonlinear rheology. The Kratky plots of SANS data demonstrate the presence of small cross-linked aggregates within the chemically-crosslinked network, whereas in the physically-crosslinked gels a relatively homogeneous structure is observed. Through model fitting to the scattering data, we were able to obtain structural parameters, such as correlation length (ξ), cross-sectional polymer chain radius (Rc), and the fractal dimension (df) of the gel networks. The fractal dimension df obtained from the SANS data of the physically-crosslinked and chemically crosslinked gels is 1.31 and 1.53, respectively. These values are in excellent agreement with the ones obtained from a generalized non-linear elastic theory we used to fit our stress-strain curves. The chemical crosslinking that generates coils and aggregates hinders the free stretching of the triple helices bundles in the physically-crosslinked gels.