Issue 4, 2019

Chemical and photochemical DNA “gears” reversibly control stiffness, shape-memory, self-healing and controlled release properties of polyacrylamide hydrogels

Abstract

A new class of stimuli-responsive DNA-based polyacrylamide hydrogels is described. They consist of glucosamine–boronate ester-crosslinked polyacrylamide chains being cooperatively bridged by stimuli-responsive nucleic acids. The triggered closure and dissociation of the stimuli-responsive units lead to switchable stiffness properties of the hydrogel. One hydrogel includes glucosamine–boronate esters and K+-ion-stabilized G-quadruplex units as cooperative crosslinkers. The hydrogel bridged by the two motifs reveals high stiffness, whereas the separation of the G-quadruplex bridges by 18-crown-6-ether yields a low stiffness hydrogel. By cyclic treatment of the hydrogel with K+-ions and 18-crown-6-ether, it is reversibly cycled between high and low stiffness states. The second system involves a photo-responsive hydrogel that reveals light-induced switchable stiffness functions. The polyacrylamide chains are cooperatively crosslinked by glucosamine–boronate esters and duplex nucleic acid bridges stabilized by trans-azobenzene intercalator units. The resulting hydrogel reveals high stiffness. Photoisomerization of the trans-azobenzene units to the cis-azobenzene states results in the separation of the duplex nucleic acid bridges and the formation of a low stiffness hydrogel. The control over the stiffness properties of the hydrogel matrices by means of K+-ions/crown ether or photoisomerizable trans-azobenzene/cis-azobenzene units is used to develop shape-memory, self-healing, and controlled drug-release hydrogel materials.

Graphical abstract: Chemical and photochemical DNA “gears” reversibly control stiffness, shape-memory, self-healing and controlled release properties of polyacrylamide hydrogels

Supplementary files

Article information

Article type
Edge Article
Submitted
26 Sep 2018
Accepted
29 Okt 2018
First published
31 Okt 2018
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2019,10, 1008-1016

Chemical and photochemical DNA “gears” reversibly control stiffness, shape-memory, self-healing and controlled release properties of polyacrylamide hydrogels

X. Liu, J. Zhang, M. Fadeev, Z. Li, V. Wulf, H. Tian and I. Willner, Chem. Sci., 2019, 10, 1008 DOI: 10.1039/C8SC04292F

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