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Doubly Dynamic Hydrogel Formed by Combining Boronate Ester and Acylhydrazone Bonds.

ABSTRACT: The incorporation of double dynamic bonds into hydrogels provides an effective strategy to engineer their performance on demand. Herein, novel hydrogels were PREPARED by combining two kinetically distinct dynamic covalent bonds, boronate ester and acylhydrazone bonds, and the synergistic properties of the hydrogels were studied comprehensively. The functional diblock copolymers P(N-isopropyl acrylamide-co-N-acryloyl-3-aminophenylboronic acid)-b-(N-isopropyl acrylamide-co-diacetone acrylamide) (PAD) were prepared via reversible addition-fragmentation chain transfer (RAFT) polymerization. The hydrogel was constructed by exploiting dynamic reaction of phenyboronic acid moieties with polyvinyl alcohol (PVA) and ketone moieties with adipic dihydrazide (ADH) without any catalyst. The active boronate ester linkage endows the hydrogel with fast gelation kinetics and self-healing ability, and the stable acylhydrazone linkage can enhance the mechanical property of the hydrogel. The difference in kinetics endows that the contribution of each linkage to mechanical strength of the hydrogel can be accurately estimated. Moreover, the mechanical property of the hydrogel can be readily engineered by changing the composition and solid content, as well as by controlling the formation or dissociation of the dynamic linkages. Thus, we provide a promising strategy to design and prepare multi-responsive hydrogels with tunable properties.

SUBMITTER: Liu Y

PROVIDER: S-EPMC7077654 | biostudies-literature | 2020 Feb

REPOSITORIES: biostudies-literature

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Doubly Dynamic Hydrogel Formed by Combining Boronate Ester and Acylhydrazone Bonds.

Liu Yusheng Y Liu Yigang Y Wang Qiuxia Q Han Yugui Y Chen Hao H Tan Yebang Y

Polymers 20200221 2

The incorporation of double dynamic bonds into hydrogels provides an effective strategy to engineer their performance on demand. Herein, novel hydrogels were PREPARED by combining two kinetically distinct dynamic covalent bonds, boronate ester and acylhydrazone bonds, and the synergistic properties of the hydrogels were studied comprehensively. The functional diblock copolymers P(N-isopropyl acrylamide-co-N-acryloyl-3-aminophenylboronic acid)-b-(N-isopropyl acrylamide-co-dia ...[more]

PMID: 32098242

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Project description:Cells are capable of sensing the differences in elastic and viscous properties (i.e., the 'viscoelasticity') of their tissue microenvironment and responding accordingly by changing their transcriptional activity and modifying their behaviors. When designing viscoelastic materials to mimic the mechanical properties of native tissue niches, it is important to consider the timescales over which cells probe their microenvironment, as the response of a viscoelastic material to an imposed stress or strain is timescale dependent. Although the timescale of cellular mechano-sensing is currently unknown, hydrogel substrates with tunable viscoelastic spectra can allow one to probe the cellular response to timescale dependent mechanical properties. Here, we report on a cytocompatible and viscoelastic hydrogel culture system with reversible boronate ester cross-links, formed from pendant boronic acid and vicinal diol moieties, where the equilibrium kinetics of esterification were leveraged to tune the viscoelastic spectrum. We found that viscoelasticity increased as a function of the boronic acid and vicinal diol concentration, and also increased with decreasing cross-linker concentration, where the maximal loss tangent achieved with this system was 0.55 at 0.1 rad s-1. Additionally, we found that the cis-vicinal diols configuration altered the viscoelastic spectra, where a tan δ peak occurred at ~1 rad s-1 for hydrogels functionalized with boronic acid, while an additional peak formed at ≥10 rad s-1 for hydrogels functionalized with both boronic acid and cis-vic-diols. In experiments with NIH-3T3 fibroblasts cultured on these hydrogels, the projected cell area and nuclear area, focal adhesion tension, and subcellular localization of YAP/TAZ were all found to be lower for cells cultured on the viscoelastic hydrogels compared to elastic hydrogels with a similar storage modulus. Despite these differences, there was not a statistically significant relationship between the frequency dependent viscoelastic material properties characterized in this study and cellular morphologies, focal adhesion tension, or the subcellular localization of YAP. While these results demonstrate that mechanotransduction pathways are affected by viscoelasticity, they also suggest that these mechanotransduction pathways are not particularly sensitive to the frequency dependent viscoelastic material properties from 0.1 to 10 rad s-1.

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Doubly Dynamic Hydrogel Formed by Combining Boronate Ester and Acylhydrazone Bonds.

Publications

Doubly Dynamic Hydrogel Formed by Combining Boronate Ester and Acylhydrazone Bonds.

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