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.

Self-healing gels based on constitutional dynamic chemistry and their potential applications

During the last decade or two the interest towards small molecules capable of self-assembly leading to gelation has increased intensively The investigation of these supramolecular gels aims not only at understanding the fundamental processes underlying gel formation but also at development of new materials with a myriad of applications Steroids are widely-spread natural products with a large and rigid steroidal nucleus combined with derivatizable functional groups leading to an adjustable polarity profile, which makes them attractive building blocks when designing novel low molecular weight gelators Due to their unique properties, steroid-based supramolecular gels may find use in applications ranging from materials science and nanoelectronics to their application as reaction media or as sensing and responsive materials Moreover, biomaterials based on steroidal gels may find use in biomedicine, drug delivery, regenerative medicine, and tissue engineering This article summarizes the most recent advances in the field of steroidal supramolecular gels in terms of steroid-derived hydro- and organogels, metallogels, two-component gels, and stimuli-responsive gels Furthermore, the potential applications of the systems are discussed

Recent advances in steroidal supramolecular gels

A dextran-based self-healing hydrogel is prepared by reversible Diels-Alder reaction under physiological conditions. Cytocompatible fulvene-modified dextran as main polymer chains and dichloromaleic-acid-modified poly(ethylene glycol) as cross-linkers are used. Both macro- and microscopic observation as well as the rheological recovery test confirm the self-healing property of the dextran-l-poly(ethylene glycol) hydrogels ("l" means "linked-by"). In addition, scanning electrochemical microscopy is used to qualitatively and quantitatively in situ track the self-healing process of the hydrogel for the first time. It is found that the longitudinal depth of scratch on hydrogel surface almost completely healed at 37 °C after 7 h. This work represents a facile approach for fabrication of polysaccharide self-healing hydrogel, which can be potentially used in several biomedical fields.

Dextran-based self-healing hydrogels formed by reversible diels-alder reaction under physiological conditions.

A distinct and well-defined nano/micro-ring structure has been obtained from the gelation process in an asymmetric peptide-based organogel. The size of the ring can be tuned in a facile manner by varying the concentration and solvent of the gel, as well as with a sonication stimulus. The gel responds to mechanical stimulus by the ring separating into a biased arc structure to expel the solvent molecules from the gel network, resulting in a gel to sol transition. The gel can self-heal again after resting and this process is reversible many times. Thus a reversible rheological switch upon alternate shaking and resting is performed via the distinct ring disintegration and reconstitution of the gel network. It was interesting to note that the gelation also takes place by a simple shaking–resting process in a solvent/solid system at room temperature without a heating–cooling process.

/pdf/thixotropic-and-self-healing-triggered-reversible-rheology-2bkjobg971.pdf

Thixotropic and self-healing triggered reversible rheology switching in a peptide-based organogel with a cross-linked nano-ring pattern

Enhanced dual network hydrogels consisting of thiolated chitosan and silk fibroin for cartilage tissue engineering.

Three novel LS2-type dimeric-cholesteryl derivatives (1–3), where S is a steroidal residue and L stands for a linker connecting the two S residues and contains three benzene rings and two amide and...

Novel dimeric cholesteryl derivatives and their smart thixotropic gels.

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Novel dimeric cholesteryl derivatives and their smart thixotropic gels.