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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.

SUBMITTER: Liu X

PROVIDER: S-EPMC6346408 | biostudies-literature | 2019 Jan

REPOSITORIES: biostudies-literature

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

Liu Xia X Zhang Junji J Fadeev Michael M Li Ziyuan Z Wulf Verena V Tian He H Willner Itamar I

Chemical science 20181031 4

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<sup>+</sup>-ion-stabilized G-quadruplex units as cooperative crosslinkers. The hydrogel bri ...[more]

PMID: 30774895

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Project description:Photoresponsive nucleic acid-based carboxymethyl cellulose (CMC) hydrogels are synthesized, and their application as shape-memory and self-healing functional matrices are discussed. One system involves the preparation of a carboxymethyl cellulose hydrogel crosslinked by self-complementary nucleic acid duplexes and by photoresponsive trans-azobenzene/?-cyclodextrin (?-CD) supramolecular complexes. Photoisomerization of the trans-azobenzene to the cis-azobenzene results in a hydrogel exhibiting lower stiffness due to the separation of the azobenzene/?-CD bridging units. The hydrogel is switched between high and low stiffness states by the cyclic and reversible light-induced isomerization of the azobenzene units between the trans and cis states. The light-controlled stiffness properties of the hydrogel are used to develop a shape-memory hydrogel, where the duplex bridging units act as permanent memory in the quasi-liquid shapeless state of the hydrogel. A second system in the study is a carboxymethyl cellulose hydrogel crosslinked by the K+-stabilized G-quadruplex bridging units and by trans-azobenzene/?-CD complexes. The resulting hydrogel includes dual-trigger functionalities, where the trans-azobenzene/?-CD complexes can be reversibly formed and dissociated through the trans and cis photoisomerization of the azobenzene units, and the K+-stabilized G-quadruplexes can be reversibly dissociated and reformed in the presence of 18-crown-6-ether/K+-ions. The signal-responsive crosslinked hydrogel reveals controlled stiffness properties, where the hydrogel crosslinked by the trans-azobenzene/?-CD and K+-ion-stabilized G-quadruplex reveals high stiffness and the hydrogel crosslinked only by the K+-ion-stabilized G-quadruplexes or only by the trans-azobenzene/?-CD complexes reveals low stiffness properties. The controlled stiffness properties of the hydrogel are used to develop shape-memory hydrogels, where the trans-azobenzene/?-CD complexes or the K+-ion-stabilized G-quadruplexes act as permanent memories in the shapeless and quasi-liquid states of the hydrogels. In addition, the hydrogel that includes two types of stimuli-responsive crosslinking units is used as a self-healing matrix, where each of the triggers guides the self-healing processes.

Dataset Information

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

Publications

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

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