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      Injectable self-healing hydrogels formed via thiol/disulfide exchange of thiol functionalized F127 and dithiolane modified PEG

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          Abstract

          An injectable thermo-responsive hydrogel with excellent mechanical properties which can self-heal under mildly acidic to basic conditions was prepared.

          Abstract

          Injectable self-healing hydrogels have found broad applications in drug delivery, tissue engineering and controlled 3D cell culture. Recently, cyclic disulfides were found to be useful in cross-linking and stabilizing liposomes by disulfide exchange polymerization, benefiting from the enhanced reactivity of the disulfide bonds. Herein, we report an injectable self-healing hydrogel constructed from cross-linked F127 with thermo and pH dual responsivity. The rapid sol–gel transition ability at body temperature allows it to be used as an injectable hydrogel. And the increased reactivity of the disulfides of cyclic dithiolane due to the ring tension makes the hydrogel self-heal under not only alkaline conditions but also neutral or even mildly acidic conditions.

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          Covalent adaptable networks: smart, reconfigurable and responsive network systems.

          Christopher J. Kloxin, Christopher Bowman (2013)
          Covalently crosslinked materials, classically referred to as thermosets, represent a broad class of elastic materials that readily retain their shape and molecular architecture through covalent bonds that are ubiquitous throughout the network structure. These materials, in particular in their swollen gel state, have been widely used as stimuli responsive materials with their ability to change volume in response to changes in temperature, pH, or other solvent conditions and have also been used in shape memory applications. However, the existence of a permanent, unalterable shape and structure dictated by the covalently crosslinked structure has dramatically limited their abilities in this and many other areas. These materials are not generally reconfigurable, recyclable, reprocessable, and have limited ability to alter permanently their stress state, topography, topology, or structure. Recently, a new paradigm has been explored in crosslinked polymers - that of covalent adaptable networks (CANs) in which covalently crosslinked networks are formed such that triggerable, reversible chemical structures persist throughout the network. These reversible covalent bonds can be triggered through molecular triggers, light or other incident radiation, or temperature changes. Upon application of this stimulus, rather than causing a temporary shape change, the CAN structure responds by permanently adjusting its structure through either reversible addition/condensation or through reversible bond exchange mechanisms, either of which allow the material to essentially reequilibrate to its new state and condition. Here, we provide a tutorial review on these materials and their responsiveness to applied stimuli. In particular, we review the broad classification of these materials, the nature of the chemical bonds that enable the adaptable structure, how the properties of these materials depend on the reversible structure, and how the application of a stimulus causes these materials to alter their shape, topography, and properties.
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            Self-healing gels based on constitutional dynamic chemistry and their potential applications.

            Miklos Zrinyi, Patrick Dussault, Yoshihito Osada … (2014)
            As representative soft materials with widespread applications, gels with various functions have been developed. However, traditional gels are vulnerable to stress-induced formation of cracks. The propagation of these cracks may affect the integrity of network structures of gels, resulting in the loss of functionality and limiting the service life of the gels. To address this challenge, self-healing gels that can restore their functionalities and structures after damage have been developed as "smart" soft materials. In this paper, we present an overview of the current strategies for synthesizing self-healing gels based on the concept of constitutional dynamic chemistry, which involves molecular structures capable of establishing dynamic networks based upon physical interactions or chemical reactions. The characterization methods of self-healing gels and the key factors that affect self-healing properties are analyzed. We also illustrate the emerging applications of self-healing gels, with emphasis on their usage in industry (coatings, sealants) and biomedicine (tissue adhesives, agents for drug or cell delivery). We conclude with a perspective on challenges facing the field, along with prospects for future development.
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              In situ gelling stimuli-sensitive block copolymer hydrogels for drug delivery.

              Ji C. He, S. H. Kim, Christopher S D Lee (2008)
              Stimuli-sensitive block copolymer hydrogels, which are reversible polymer networks formed by physical interactions and exhibit a sol-gel phase-transition in response to external stimuli, have great potential in biomedical and pharmaceutical applications, especially in site-specific controlled drug-delivery systems. The drug may be mixed with a polymer solution in vitro and the drug-loaded hydrogel can form in situ after the in vivo administration, such as injection; therefore, stimuli-sensitive block copolymer hydrogels have many advantages, such as simple drug formulation and administration procedures, no organic solvent, site-specificity, a sustained drug release behavior, less systemic toxicity and ability to deliver both hydrophilic and hydrophobic drugs. Among the stimuli in the biomedical applications, temperature and pH are the most popular physical and chemical stimuli, respectively. The temperature- and/or pH-sensitive block copolymer hydrogels for biomedical applications have been extensively developed in the past decade. This review focuses on recent development of the preparation and application for drug delivery of the block copolymer hydrogels that respond to temperature, pH or both stimuli, including poly(N-substituted acrylamide)-based block copolymers, poloxamers and their derivatives, poly(ethylene glycol)-polyester block copolymers, polyelectrolyte-based block copolymers and the polyelectrolyte-modified thermo-sensitive block copolymers. In addition, the hydrogels based on other stimuli-sensitive block copolymers are discussed.
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                Author and article information

                Contributors
                Journal
                Journal ID (publisher-id): JMCBDV
                Title: Journal of Materials Chemistry B
                Abbreviated Title: J. Mater. Chem. B
                Publisher: Royal Society of Chemistry (RSC)
                ISSN (Print): 2050-750X
                ISSN (Electronic): 2050-7518
                Publication date Created: 2017
                Publication date (Electronic): 2017
                Volume: 5
                Issue: 22
                Pages: 4121-4127
                Affiliations
                [1 ]CAS Key Laboratory of Soft Matter Chemistry
                [2 ]School of Chemistry and Materials Science
                [3 ]University of Science and Technology of China
                [4 ]Hefei
                [5 ]P. R. China
                Article
                DOI: 10.1039/C7TB00746A
                PubMed ID: 32264144
                SO-VID: 60b8d2e9-7dcd-440a-b4c2-4791ca324cc4
                Copyright © © 2017
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