Interpenetrating polymer network (IPN) hydrogels have been subjected to more attention due to their efficacy in biomedical applications. Comparing to single network hydrogels, interpenetrated networks possess distinct properties such as high fracture strain and high compressive strength. Spatial control of these properties can lead to potential applications in drug delivery as well as tissue engineering. In this work a temporal control of mechanical property was achieved using carbodiimides hydration as the fuel reaction. Carbodiimide hydration can be used to link carboxylic acids as anhydrides. The hydration of carbodiimides can be applied to prepare transient polymer networks. A semi-IPN was synthesized using a carboxylic-acid-functionalized free polymer poly(Amx-AA100-x) and a permanent covalent crosslinked polymer Poly(Amx-AA100-x-MBAM1.3). In the presence of 1-ethyl-3-(3-dimethylaminopropyl)carbodiimide (EDC), anhydride crosslinks were formed by carboxylic acid pendant groups resulting an IPN which eventually returns to the resting state by hydrolysis. The characterization of the hydrogels in unfueled, fueled, resting and refueled states were done using fracture energy test. The effect of polymer architecture on fracture energy of fueled IPNs was also analyzed. Additionally, IPN fueled with EDC has higher resistance for compression when compared to single network polymer hydrogels. Various kirigami type patterns were also designed.

Carbodiimide fuels create transient tough interpenetrated networks

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