.png){kind=icon}
.png){kind=icon}
Return
Force-Triggered Self-Destructive Hydrogels
.png){kind=icon}
OA
AI
DOI：10.1002/adma.202305544.png)
.png){kind=icon}
Original request for help.png){kind=icon}
Share.png){kind=icon}
Save
Abstract
En 中文
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, no known SDPs that respond to external mechanical forces have 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, the development of force-triggered SDPs composed of DNA crosslinked hydrogels doped with nucleases is described here. Externally applied piconewton forces selectively expose enzymatic cleavage sites within the DNA crosslinks, resulting in rapid polymer self-degradation. The synthesis and the chemical and mechanical characterization of DNA crosslinked hydrogels, as well as the kinetics of force-triggered hydrolysis, are described. As a proof-of-concept, force-triggered and time-dependent rheological changes in the polymer as well as encapsulated nanoparticle release are demonstrated. Finally, that the kinetics of self-destruction are shown to be tuned as a function of nuclease concentration, incubation time, and thermodynamic stability of DNA crosslinkers. Force-triggered self-destructive hydrogels are developed by using mechano-responsive DNA hairpins that crosslink the gel network. The DNA is protected by folding under static conditions, but under force, cryptic sites are exposed, which allows Cas12a nuclease to destroy the phosphodiester DNA backbone. In this work, tunable force sensitivity is demonstrated to trigger self-destruction and cargo release from the hydrogel.image
Keywords:
CRISPR Cas12a
DNA hairpins
mechanically induced depolymerization
responsive hydrogels
rheology
self-destructive