Force Trigged Self-destructive Hydrogels.

Self-Destructive Polymers (SDPs) are defined as a class of smart polymers that autonomously degrade upon experiencing an external trigger, such as a chemical cue or optical excitation. Because SDPs release the materials trapped inside the network upon degradation, they have potential applications in drug delivery and analytical sensing. However, to the best of our knowledge, SDPs that respond to external mechanical forces have not been reported, as it is fundamentally challenging to create mechano-sensitivity in general and especially so for force levels below those required for classical force-induced bond scission. To address this challenge, we describe the development of force-triggered SDPs comprised of DNA crosslinked hydrogels doped with nucleases. Externally-applied piconewton forces selectively expose enzymatic cleavage sites within the DNA crosslinks, resulting in rapid polymer self-degradation. We describe the synthesis, chemical and mechanical characterization of DNA crosslinked hydrogels, as well as the kinetics of force-triggered hydrolysis. As a proof-of-concept, we also demonstrate force-triggered and time-dependent rheological changes in the polymer as well as encapsulated nanoparticle release. Finally, we show that the kinetics of self-destruction can be tuned as a function of nuclease concentration, incubation time, and the thermodynamic stability of DNA crosslinkers. This article is protected by copyright. All rights reserved.