Thermoresponsive poly(N-isopropylacrylamide) (PNIPAAm) hydrogels are widely studied smart materials, particularly for biomedical applications, but are limited by their mechanical strength. In this study, double network (DN) hydrogels were prepared with an asymmetric crosslink design and inclusion of an electrostatic co-monomer, 2-acrylamido-2-methylpropane sulfonic acid (AMPS). These P(NIPAAm-co-AMPS)/PNIPAAm DN hydrogels were sequentially formed with a tightly crosslinked 1st network comprised of variable levels of AMPS (100 : 0 to 25 : 75 wt% ratio of NIPAAm:AMPS) and a loosely crosslinked 2nd network comprised of PNIPAAm. The impact of AMPS content in the 1st network on the volume phase transition temperature (VPTT), morphology, deswelling–reswelling kinetics and mechanical properties was evaluated. Without substantially altering the VPTT of conventional PNIPAAm hydrogels but with improving thermosensitivity, the DN hydrogel formed with 25 : 75 wt% of NIPAAm:AMPS achieved exceptional strength, high modulus and high %strain at break.
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