The molecular origin of enhanced toughness in double-network hydrogels: A neutron scattering study

Double-network hydrogels (DN-gels) are a new class of crosslinked polymer networks with extraordinary mechanical properties while containing 80-90 vol.% water. Small-angle neutron scattering (SANS) was applied to investigate the molecular origin of the mechanical properties observed in DN-gels. We present SANS results in both deformed and undeformed conditions for a tough DN-gel made of poly(2-acrylamido-2-methyl-1-propane sulfonic acid) (PAMPS) and polyacrylamide (PAAm). The SANS measurements indicate that deformation of DN-gels results in periodic and mesoscale (∼1.5 μm) compositional fluctuations in both PAMPS and PAAm. In addition, SANS measurements also indicate that the DN-gel constituents interact favorably with each other while in water. This favorable interaction between PAMPS and PAAm is consistent with the rheological results on solution mixtures of these two polymers. The implications of the above observations to toughening mechanisms are discussed.