Hydrogels Based on Dynamic Covalent Chemistry

A special issue of Gels (ISSN 2310-2861).

Deadline for manuscript submissions: closed (31 July 2017) | Viewed by 24888

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CIDETEC Parque Científico y Tecnológico de Gipuzkoa Pº Miramón, 196, 20014 Donostia-San Sebastian, Spain
Interests: dynamic hydrogels; stimuli-responsive materials; colloids; emulsions; biomaterials; tissue engineering; wound healing; drug delivery; rheology
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Special Issue Information

Dear Colleagues,

A Special Issue on “Hydrogels Based on Dynamic Covalent Chemistry” is a perfect window to advertise scientific efforts on the design and characterization of this new type of hydrogels scarcely reported, so far, in the literature, but that are related to various areas, such as soft matter, biomaterials, tissue engineering, and drug delivery.

Conventional hydrogels, either covalent or physical, are considered as static 3D networks with constant rheological and mechanical properties. The incorporation of reversible covalent bonds, such as [phenylboronate–salicylhydroxamate] reaction, boronic ester bonds, and thiol/disulfide exchange among others, in polymeric network offers a new approach to design hydrogels with dynamic properties. First, the functionalization of polymeric material with such functionalities implies novel synthetic strategies. In addition, the continuous reversible reaction allows the permanent movement of the network, which results in peculiar properties for the resulting hydrogel. While the dynamic behaviour is often related to the self-healing ability of the 3D network, the “moving network” results in particular mechanical properties like frequency dependent stiffness, also called shock absorbing properties. Although this property has been attributed to the kinetic of the reversible covalent bond, mathematical modelisation is still missing to confirm the experimental observation. Interestingly, the stiffness of dynamic hydrogels can be easily tuned from highly viscous material to very hard free-standing hydrogels. All those new hydrogels have the particularity to be injected and reshaped indefinitely, which make them potential candidate as biomaterial for tissue engineering and drug delivery systems.

Dr. Damien Dupin
Guest Editor

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Keywords

  • reversible covalent bond
  • dynamic hydrogels
  • self-healing
  • rheology
  • mechanical properties
  • relaxation time
  • frequency-dependent stiffness
  • biomaterials
  • scaffold

Published Papers (4 papers)

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Research

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3352 KiB  
Article
Exploration of Dynamic Elastic Modulus Changes on Glioblastoma Cell Populations with Aberrant EGFR Expression as a Potential Therapeutic Intervention Using a Tunable Hyaluronic Acid Hydrogel Platform
by Hemamylammal Sivakumar, Roy Strowd and Aleksander Skardal
Gels 2017, 3(3), 28; https://doi.org/10.3390/gels3030028 - 13 Jul 2017
Cited by 15 | Viewed by 4926
Abstract
Glioblastoma (GBM) is one of most aggressive forms of brain cancer, with a median survival time of 14.6 months following diagnosis. This low survival rate could in part be attributed to the lack of model systems of this type of cancer that faithfully [...] Read more.
Glioblastoma (GBM) is one of most aggressive forms of brain cancer, with a median survival time of 14.6 months following diagnosis. This low survival rate could in part be attributed to the lack of model systems of this type of cancer that faithfully recapitulate the tumor architecture and microenvironment seen in vivo in humans. Therapeutic studies would provide results that could be translated to the clinic efficiently. Here, we assess the role of the tumor microenvironment physical parameters on the tumor, and its potential use as a biomarker using a hyaluronic acid hydrogel system capable of elastic modulus tuning and dynamic elastic moduli changes. Experiments were conducted to assess the sensitivity of glioblastoma cell populations with different mutations to varying elastic moduli. Cells with aberrant epithelial growth factor receptor (EGFR) expression have a predilection for a stiffer environment, sensing these parameters through focal adhesion kinase (FAK). Importantly, the inhibition of FAK or EGFR generally resulted in reversed elastic modulus preference. Lastly, we explore the concept of therapeutically targeting the elastic modulus and dynamically reducing it via chemical or enzymatic degradation, both showing the capability to reduce or stunt proliferation rates of these GBM populations. Full article
(This article belongs to the Special Issue Hydrogels Based on Dynamic Covalent Chemistry)
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5537 KiB  
Article
Nanoparticulate Poly(glucaramide)-Based Hydrogels for Controlled Release Applications
by Erik R. Johnston, Tyler N. Smith and Monica A. Serban
Gels 2017, 3(2), 17; https://doi.org/10.3390/gels3020017 - 06 May 2017
Cited by 1 | Viewed by 4415
Abstract
In 2004, D-Glucaric acid (GA) was identified as one of the top value-added chemicals from renewable feedstocks. For this study, a patented synthetic method was used to obtain gel forming polymers through the polycondensation of GA and several aliphatic diamines. The first time [...] Read more.
In 2004, D-Glucaric acid (GA) was identified as one of the top value-added chemicals from renewable feedstocks. For this study, a patented synthetic method was used to obtain gel forming polymers through the polycondensation of GA and several aliphatic diamines. The first time characterization and a potential practical application of such hydrogels is reported herein. Our findings indicate that the physical properties and gelling abilities of these materials correlate with the chemical structure of the precursor diamines used for polymerization. The hydrogels appear to have nanoparticulate nature, form via aggregation, are thermoresponsive, and appear suitable as controlled release systems for small molecules. Overall, this study further highlights the versatility of GA as a building block for the synthesis of sustainable materials, with potential for a wide array of applications. Full article
(This article belongs to the Special Issue Hydrogels Based on Dynamic Covalent Chemistry)
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Review

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11 pages, 2215 KiB  
Review
Hydrogels Based on Dynamic Covalent and Non Covalent Bonds: A Chemistry Perspective
by Francesco Picchioni and Henky Muljana
Gels 2018, 4(1), 21; https://doi.org/10.3390/gels4010021 - 08 Mar 2018
Cited by 55 | Viewed by 7948
Abstract
Hydrogels based on reversible covalent bonds represent an attractive topic for research at both academic and industrial level. While the concept of reversible covalent bonds dates back a few decades, novel developments continue to appear in the general research area of gels and [...] Read more.
Hydrogels based on reversible covalent bonds represent an attractive topic for research at both academic and industrial level. While the concept of reversible covalent bonds dates back a few decades, novel developments continue to appear in the general research area of gels and especially hydrogels. The reversible character of the bonds, when translated at the general level of the polymeric network, allows reversible interaction with substrates as well as responsiveness to variety of external stimuli (e.g., self-healing). These represent crucial characteristics in applications such as drug delivery and, more generally, in the biomedical world. Furthermore, the several possible choices that can be made in terms of reversible interactions generate an almost endless number of possibilities in terms of final product structure and properties. In the present work, we aim at reviewing the latest developments in this field (i.e., the last five years) by focusing on the chemistry of the systems at hand. As such, this should allow molecular designers to develop a toolbox for the synthesis of new systems with tailored properties for a given application. Full article
(This article belongs to the Special Issue Hydrogels Based on Dynamic Covalent Chemistry)
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11111 KiB  
Review
Peptide-Based Physical Gels Endowed with Thixotropic Behaviour
by Nicola Zanna and Claudia Tomasini
Gels 2017, 3(4), 39; https://doi.org/10.3390/gels3040039 - 21 Oct 2017
Cited by 24 | Viewed by 6388
Abstract
Thixotropy is one of the oldest documented rheological phenomenon in colloid science and may be defined as an increase of viscosity in a state of rest and a decrease of viscosity when submitted to a constant shearing stress. This behavior has been exploited [...] Read more.
Thixotropy is one of the oldest documented rheological phenomenon in colloid science and may be defined as an increase of viscosity in a state of rest and a decrease of viscosity when submitted to a constant shearing stress. This behavior has been exploited in recent years to prepare injectable hydrogels for application in drug delivery systems. Thixotropic hydrogels may be profitably used in the field of regenerative medicine, which promotes tissue healing after injuries and diseases, as the molten hydrogel may be injected by syringe and then self-adapts in the space inside the injection site and recovers the solid form. We will focus our attention on the preparation, properties, and some applications of biocompatible thixotropic hydrogels. Full article
(This article belongs to the Special Issue Hydrogels Based on Dynamic Covalent Chemistry)
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