Self-Healing Hydrogels for Applications in Regenerative Medicine

A special issue of Gels (ISSN 2310-2861). This special issue belongs to the section "Gel Applications".

Deadline for manuscript submissions: closed (30 April 2023) | Viewed by 19961

Special Issue Editors


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Guest Editor
Key State Laboratory of Fine Chemicals, School of Bioengineering, Dalian University of Technology, Dalian 116024, China
Interests: self-healing hydrogels; tissue engineering; adhesive hydrogels; colloidal gels; 3D bioprinting; microfluidic droplets
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Guest Editor
School of Materials Science and Engineering, South China University of Technology, Guangzhou 510640, China
Interests: supramolecular hydrogels; adhesives; emulsions; tissue engineering

Special Issue Information

Dear Colleagues,

Organisms in nature have shown fascinating abilities with respect to self-healing and regenerating their structural and functional properties after damages caused by trauma or diseases. This outstanding self-management of damage is the most important source of inspiration for the design and engineering of materials capable of reversing damage development. Inspired by this concept, Scott White and Nancy Sottos first reported the discovery of self-healing materials in 2001, thus opening a new era in materials science and engineering. Following this finding, self-healing hydrogels have been developed, which are hydrophilic polymer networks that, after damage, can revert to their original state with full or partial recovery of mechanical strength. Due to the resemblance with extracellular matrices of tissue/organs, hydrogels capable of self-recovery are expected to be candidate materials for applications in regenerative medicine. Indeed, the past decade has witnessed the development of self-healing gels for applications in tissue engineering, controlled drug/cell delivery, injectable defect filler materials, and 3D bioprinting, which can be attributed to their special viscoelastic properties and mechanical durability. In this Special Issue, we will focus on recent progress in the design of self-healing hydrogels for biomedical applications. We will discuss the potential use of self-healing gels for different fields of tissue regenerations. In particular, we envision the future directions of this research area to proliferate the development of practically useful self-healing materials and their recent applications in regenerative medicine. We look forward to the submission of new results on self-healing gels and its recent applications in regenerative medicine.

Prof. Dr. Huanan Wang
Prof. Dr. Yunhua Chen
Guest Editors

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Keywords

  • Self-healing
  • Hydrogels
  • Reversible crosslinking
  • Shear-thinning
  • Regenerative Medicine
  • Cell-based therapy
  • 3D Bioprinting

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Related Special Issue

Published Papers (5 papers)

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Research

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31 pages, 8071 KiB  
Article
Self-Healing and Super-Elastomeric PolyMEA-co-SMA Nanocomposites Crosslinked by Clay Platelets
by Beata Strachota, Adam Strachota, Katarzyna Byś, Ewa Pavlova, Jiří Hodan and Beata Mossety-Leszczak
Gels 2022, 8(10), 657; https://doi.org/10.3390/gels8100657 - 15 Oct 2022
Cited by 2 | Viewed by 1942
Abstract
Novel solvent-free ultra-extensible, tough, and self-healing nanocomposite elastomers were synthesized. The self-assembled materials were based on the copolymer matrix poly(methoxyethyl acrylate-co-sodium methacrylate) physically crosslinked by clay nano-platelets (‘poly[MEA-co-SMA]/clay’). Depending on the content of SMA, the super-elastomers were predominantly hydrophobic, water-swelling, or fully water-soluble, [...] Read more.
Novel solvent-free ultra-extensible, tough, and self-healing nanocomposite elastomers were synthesized. The self-assembled materials were based on the copolymer matrix poly(methoxyethyl acrylate-co-sodium methacrylate) physically crosslinked by clay nano-platelets (‘poly[MEA-co-SMA]/clay’). Depending on the content of SMA, the super-elastomers were predominantly hydrophobic, water-swelling, or fully water-soluble, and hence repeatedly processible. The SMA co-monomer introduces a tremendous increase in tensile strength, an increase in toughness, while ultra-extensibility is preserved. By tuning the contents of nano-clay and SMA co-monomer, a very wide range of product properties was achieved, including extreme ultra-extensibility, or high stiffness combined with more moderate super-extensibility, or very different values of tensile strength. There was very attractive, great improvement in autonomous self-healing ability induced by SMA, combined with tremendously enhanced self-recovery of internal mechanical damage: even complete self-recovery could be achieved. The ionic SMA repeat units were found to assemble to multiplets, which are phase-separated in the hydrophobic polyMEA matrix. The dynamics of SMA-units-hopping between these aggregates was of key importance for the mechanical, visco-elastic, tensile, and self-healing properties. The studied super-elastomers are attractive as advanced self-healing materials in engineering, soft robotics, and in medical or implant applications. Full article
(This article belongs to the Special Issue Self-Healing Hydrogels for Applications in Regenerative Medicine)
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11 pages, 3442 KiB  
Article
Compliant, Tough, Anti-Fatigue, Self-Recovery, and Biocompatible PHEMA-Based Hydrogels for Breast Tissue Replacement Enabled by Hydrogen Bonding Enhancement and Suppressed Phase Separation
by Hongyan Ouyang, Xiangyan Xie, Yuanjie Xie, Di Wu, Xingqi Luo, Jinrong Wu, Yi Wang and Lijuan Zhao
Gels 2022, 8(9), 532; https://doi.org/10.3390/gels8090532 - 25 Aug 2022
Cited by 2 | Viewed by 2132
Abstract
Although hydrogel is a promising prosthesis implantation material for breast reconstruction, there is no suitable hydrogel with proper mechanical properties and good biocompatibility. Here, we report a series of compliant and tough poly (hydroxyethyl methacrylate) (PHEMA)-based hydrogels based on hydrogen bond-reinforcing interactions and [...] Read more.
Although hydrogel is a promising prosthesis implantation material for breast reconstruction, there is no suitable hydrogel with proper mechanical properties and good biocompatibility. Here, we report a series of compliant and tough poly (hydroxyethyl methacrylate) (PHEMA)-based hydrogels based on hydrogen bond-reinforcing interactions and phase separation inhibition by introducing maleic acid (MA) units. As a result, the tensile strength, fracture strain, tensile modulus, and toughness are up to 420 kPa, 293.4%, 770 kPa, and 0.86 MJ/m3, respectively. Moreover, the hydrogels possess good compliance, where the compression modulus is comparable to that of the silicone breast prosthesis (~23 kPa). Meanwhile, the hydrogels have an excellent self-recovery ability and fatigue resistance: the dissipative energy and elastic modulus recover almost completely after waiting for 2 min under cyclic compression, and the maximum strength remains essentially unchanged after 1000 cyclic compressions. More importantly, in vitro cellular experiments and in vivo animal experiments demonstrate that the hydrogels have good biocompatibility and stability. The biocompatible hydrogels with breast tissue-like mechanical properties hold great potential as an alternative implant material for reconstructing breasts. Full article
(This article belongs to the Special Issue Self-Healing Hydrogels for Applications in Regenerative Medicine)
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23 pages, 7003 KiB  
Article
Mucoadhesive and Antimicrobial Allantoin/β Cyclodextrins-Loaded Carbopol Gels as Scaffolds for Regenerative Medicine
by Daniela Filip, Doina Macocinschi, Mirela-Fernanda Zaltariov, Carmen Anatolia Gafitanu, Cristina Gabriela Tuchilus, Adrian Bele, Bianca-Iulia Ciubotaru, Elena Stoleru and Alexandra Bargan
Gels 2022, 8(7), 416; https://doi.org/10.3390/gels8070416 - 2 Jul 2022
Cited by 7 | Viewed by 2494
Abstract
Allantoin and its β-cyclodextrin and hydroxypropyl-β-cyclodextrin inclusion complexes 1:1 have been used to prepare carbopol-based mucoadhesive gels. The gelation process occurred by adjustment with glycerol 10% in the presence of triethanolamine. The structural features induced by the presence of allantoin and the corresponding [...] Read more.
Allantoin and its β-cyclodextrin and hydroxypropyl-β-cyclodextrin inclusion complexes 1:1 have been used to prepare carbopol-based mucoadhesive gels. The gelation process occurred by adjustment with glycerol 10% in the presence of triethanolamine. The structural features induced by the presence of allantoin and the corresponding β-cyclodextrins inclusion complexes have been first investigated by infrared spectroscopy highlighting strong interactions within the gels network and ideal crosslinks for the self-healing behavior. The hydrophilicity of the gels was investigated by the determination of the surface tension parameters and the free energy of hydration. The interfacial free energy values indicated prolonged biocompatibility with blood. The gels-water molecule interactions in terms of sorption, permeability, and diffusion coefficients were evaluated by dynamic vapor sorption analysis. The self-assembly process through intermolecular H-bonding, the high hydrophilicity, the mechanical performance, the hydrolytic stability in simulated biological media, the biocompatibility with normal human dermal fibroblast (NHDF) cells, the mucoadhesivity and antimicrobial activity on selected microorganism species (S. Aureus and C. albicans) of the allantoin-based gels recommend them as promising scaffold alternatives in regenerative medicine. Full article
(This article belongs to the Special Issue Self-Healing Hydrogels for Applications in Regenerative Medicine)
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12 pages, 2116 KiB  
Article
A Supramolecular Hydrogel Enabled by the Synergy of Hydrophobic Interaction and Quadruple Hydrogen Bonding
by Liangmei Lu, Wen Zhou, Zhuzuan Chen, Yang Hu, Yu Yang, Guangzhao Zhang and Zhuohong Yang
Gels 2022, 8(4), 244; https://doi.org/10.3390/gels8040244 - 14 Apr 2022
Cited by 14 | Viewed by 3519
Abstract
The increasing preference for minimally invasive surgery requires novel soft materials that are injectable, with rapid self-healing abilities, and biocompatible. Here, by utilizing the synergetic effect of hydrophobic interaction and quadruple hydrogen bonding, an injectable supramolecular hydrogel with excellent self-healing ability was synthesized. [...] Read more.
The increasing preference for minimally invasive surgery requires novel soft materials that are injectable, with rapid self-healing abilities, and biocompatible. Here, by utilizing the synergetic effect of hydrophobic interaction and quadruple hydrogen bonding, an injectable supramolecular hydrogel with excellent self-healing ability was synthesized. A unique ABA triblock copolymer was designed containing a central poly(ethylene oxide) block and terminal poly(methylmethacrylate) (PMMA) block, with ureido pyrimidinone (UPy) moieties randomly incorporated (termed MA-UPy-PEO-UPy-MA). The PMMA block could offer a hydrophobic microenvironment for UPy moieties in water and thus boost the corresponding quadruple hydrogen bonding interaction of Upy–Upy dimers. Owing to the synergetic effect of hydrophobicity and quadruple hydrogen bonding interaction, the obtained MA-UPy-PEO-UPy-MA hydrogel exhibited excellent self-healing properties, and injectable capability, as well as superior mechanical strength, and therefore, it holds great promise in tissue engineering applications, including in cell support and drug release. Full article
(This article belongs to the Special Issue Self-Healing Hydrogels for Applications in Regenerative Medicine)
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Review

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33 pages, 6685 KiB  
Review
Self-Healing Mechanism and Conductivity of the Hydrogel Flexible Sensors: A Review
by Juan Zhang, Yanen Wang, Qinghua Wei, Yanmei Wang, Mingju Lei, Mingyang Li, Dinghao Li, Longyu Zhang and Yu Wu
Gels 2021, 7(4), 216; https://doi.org/10.3390/gels7040216 - 16 Nov 2021
Cited by 30 | Viewed by 9112
Abstract
Sensors are devices that can capture changes in environmental parameters and convert them into electrical signals to output, which are widely used in all aspects of life. Flexible sensors, sensors made of flexible materials, not only overcome the limitations of the environment on [...] Read more.
Sensors are devices that can capture changes in environmental parameters and convert them into electrical signals to output, which are widely used in all aspects of life. Flexible sensors, sensors made of flexible materials, not only overcome the limitations of the environment on detection devices but also expand the application of sensors in human health and biomedicine. Conductivity and flexibility are the most important parameters for flexible sensors, and hydrogels are currently considered to be an ideal matrix material due to their excellent flexibility and biocompatibility. In particular, compared with flexible sensors based on elastomers with a high modulus, the hydrogel sensor has better stretchability and can be tightly attached to the surface of objects. However, for hydrogel sensors, a poor mechanical lifetime is always an issue. To address this challenge, a self-healing hydrogel has been proposed. Currently, a large number of studies on the self-healing property have been performed, and numerous exciting results have been obtained, but there are few detailed reviews focusing on the self-healing mechanism and conductivity of hydrogel flexible sensors. This paper presents an overview of self-healing hydrogel flexible sensors, focusing on their self-healing mechanism and conductivity. Moreover, the advantages and disadvantages of different types of sensors have been summarized and discussed. Finally, the key issues and challenges for self-healing flexible sensors are also identified and discussed along with recommendations for the future. Full article
(This article belongs to the Special Issue Self-Healing Hydrogels for Applications in Regenerative Medicine)
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