Quadruple hydrogen bonds and thermo-triggered hydrophobic interactions generate dynamic hydrogels to modulate transplanted cell retention

The supramolecular polymer hydrogels feature self-healability, adjustable mechanical strength, and thermoplasticity, which are derived from the formation of supramolecular physical interactions in the hydrogel networks, such as H-bonding interactions, [6] host-guest interactions, [7] metal-ligand coordination interactions, [8] hydrophobic interactions, [9] multiple combined interactions. [10] Among them, H-bonds are generally weak noncovalent bonds, ubiquitous in biomolecules, but their synergistic interactions can reach a strength of the covalent bond; thus it is commonly utilized in designing supramolecular tough hydrogels. [11] Our previous study suggested that supramolecular polymer hydrogels based on single amide H-bonding interaction were unstable in water, [12] because the competitive solvation of H-bond donor and acceptor in polar solvents weakens its strengthening effect. [13] Inspired by the hydrogen-bonded clusters in the secondary structure of proteins, we constructed a supramolecular poly(N-acryloyl glycinamide) (PNAGA) hydrogel whose dual amide motifs in the side chain contributed to high strengths and outstanding antiswelling ability due to strong shielding of the hydrogen-bonded microdomains from water molecule attack. [12] By utilizing Type II photoinitiated self-condensing vinyl polymerization of N-acryloyl glycinamide (NAGA), the resultant hyperbranched PNAGA hydrogels demonstrated superior mechanical performances to those of linear PNAGA counterparts owing to the higher cross-linking density of H-bonds. [14] In addition, the H-bonding interactions of dual amide motifs could also be modulated by copolymerizing other monomers, [15][16][17][18] thus achieving the versatile hydrogels with mechanical properties spanning from high strength to soft injectability, which show promising applications as 3D printed osteochondral regeneration scaffold, [16] artificial vitreous body, [17] and postoperative antiadhesion barrier. [18] Our recent study revealed that only introducing one methyl group to the double bond of NAGA could lead to a considerable decrease in mechanical strengths and an increase in room temperature autonomous self-healability of the poly(N-methacryloyl glycinamide) hydrogels (MNAGA), which was resulted from the perturbation of one methyl substitution to H-bonds. [19] The intermolecular H-bonding density heavily influences the gelation and rheological behavior of hydrogen-bonded supramolecular polymer hydrogels, thus offering a delicate pathway to tailor their physicochemical properties for meeting a specific biomedical application. Herein, one methylene spacer between two amides in the side chain of N-acryloyl glycinamide (NAGA) is introduced to generate a variant monomer, N-acryloyl alaninamide (NAAA). Polymerization of NAAA in aqueous solution affords an unprecedented ultrasoft and highly swollen supramolecular polymer hydrogel due to weakened H-bonds caused by an extra methylene spacer, which is verified by variabletemperature Fourier transform infrared (FTIR) spectroscopy and s...

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confidence: 99%

An Ultrasoft Self‐Fused Supramolecular Polymer Hydrogel for Completely Preventing Postoperative Tissue Adhesion

et al. 2021

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“…Gelatin methacryloyl (GelMA) and fluorescein isothiocyanate graft GelMA (GelMA-FITC) were synthesized according to the previous works. [20,32] CCk-8 kit was purchased from Tonkin institute of chemistry, Japan. Phosphate-buffered saline (PBS, pH = 7.4), Dulbecco's Modified Eagle's Medium (DMEM), fetal bovine serum (FBS), penicillin-streptomycin solution, live-dead staining solution were purchased from Life Technologies (Gibco, USA).…”

Section: Methodsmentioning

confidence: 99%

Macroporous Adhesive Nano‐Enabled Hydrogels Generated from Air‐in‐Water Emulsions

Xie

Zheng

et al. 2022

Macromolecular Bioscience

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Developing nanocomposite hydrogel with multi-functions including adjustable mechanical property, tissue-adhesion, and blood coagulation property to accelerate wound healing is highly desirable in surgical application. Here a macroporous adhesive nano-enabled hydrogel constructed from gelatin methacryloyl stabilized air-in-water emulsions incorporated with dopamine-grafted-gelatin (GelDA) and Laponite nanoclay is reported. The hydrogel exhibits interconnected macroporous structure. The physical/chemical cross-linked network formed among the various components contributes to the good mechanical strength of hydrogel, which could be further regulated by adjusting the concentration of Laponite nanoclay. Furthermore, the nanocomposite macroporous hydrogel is endowed with self-healing properties and tissue adhesion by the intermolecular hydrogen bonds, ionic interactions among Laponite nanoclay and polymers, as well as the catechol functional groups. The in vitro studies demonstrate that the macroporous hydrogel has good biocompatibility and could significantly reduce blood clotting time, which is expected to be applied for the rapid sealing and hemostasis of bleeding wounds.

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“…The rheological tests of the hydrogels were determined according to our previously reported method. 37 2.2. Drug Release Assay.…”

Section: Methodsmentioning

confidence: 99%

“…The DOX& D PPA-1@HDU hydrogel was prepared similarly by further addition of DOX and the D PPA-1 peptide in the solution. The rheological tests of the hydrogels were determined according to our previously reported method …”

Section: Methodsmentioning

confidence: 99%

Injectable Supramolecular Hydrogel for Locoregional Immune Checkpoint Blockade and Enhanced Cancer Chemo-Immunotherapy

Liu

Cao

Zhang

et al. 2021

ACS Appl. Mater. Interfaces

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Immunotherapy has revolutionized the therapeutic modalities of cancer treatment but is severely limited by a low objective response rate and the risk of immune-related side effects. Herein, an injectable supramolecular hydrogel is developed for local delivery of the D PPA-1 peptide (a D-peptide antagonist with a high binding affinity to programmed cell death-ligand 1 (PD-L1)) and doxorubicin (DOX). On the one hand, DOX could kill tumor cells directly and also induce immunogenic cell death to provoke the antitumor immune response. On the other hand, the D PPA-1 peptide could locoregionally block the PD-1/PD-L1 pathway to potentiate T-cell-mediated immune responses and minimize side effects. Eventually, by local injection of this supramolecular hydrogel, the synergistic cancer therapeutic effect was evaluated, showing promise in improving the objective response rate of immunotherapy and minimizing its systemic side effects.

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Quadruple hydrogen bonds and thermo-triggered hydrophobic interactions generate dynamic hydrogels to modulate transplanted cell retention

Abstract: Supramolecular dynamic hydrogels with quadruple hydrogen bonds and thermo-triggered hydrophobic interactions demonstrate a promising capability of modulating transplanted cell retention.

Cited by 42 publications

References 57 publications

An Ultrasoft Self‐Fused Supramolecular Polymer Hydrogel for Completely Preventing Postoperative Tissue Adhesion

An Ultrasoft Self‐Fused Supramolecular Polymer Hydrogel for Completely Preventing Postoperative Tissue Adhesion

Macroporous Adhesive Nano‐Enabled Hydrogels Generated from Air‐in‐Water Emulsions

Injectable Supramolecular Hydrogel for Locoregional Immune Checkpoint Blockade and Enhanced Cancer Chemo-Immunotherapy

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