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      Bioinspired Injectable Self-Healing Hydrogel Sealant with Fault-Tolerant and Repeated Thermo-Responsive Adhesion for Sutureless Post-Wound-Closure and Wound Healing

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          Highlights

          • Mussel and brown algae inspired dual-bionic bioadhesive cross-linked by dynamic bonds exhibits good self-healing capacity and sufficient adhesive strength. And the adhesive hydrogel shows temperature-dependent reversible adhesive behavior, and could achieve fault-tolerate adhesive application and repeated tissue adhesion.

          • The coordination interaction between ferric ions and protocatechualdehyde equips the hydrogel with photothermal antibacterial effect.

          • The injectable adhesive with antioxidation and good hemostatic effect shows promising application in tissue sealant and wound closure.

          Supplementary Information

          The online version contains supplementary material available at 10.1007/s40820-022-00928-z.

          Abstract

          Hydrogels with multifunctionalities, including sufficient bonding strength, injectability and self-healing capacity, responsive-adhesive ability, fault-tolerant and repeated tissue adhesion, are urgently demanded for invasive wound closure and wound healing. Motivated by the adhesive mechanism of mussel and brown algae, bioinspired dynamic bonds cross-linked multifunctional hydrogel adhesive is designed based on sodium alginate (SA), gelatin (GT) and protocatechualdehyde, with ferric ions added, for sutureless post-wound-closure. The dynamic hydrogel cross-linked through Schiff base bond, catechol-Fe coordinate bond and the strong interaction between GT with temperature-dependent phase transition and SA, endows the resulting hydrogel with sufficient mechanical and adhesive strength for efficient wound closure, injectability and self-healing capacity, and repeated closure of reopened wounds. Moreover, the temperature-dependent adhesive properties endowed mispositioning hydrogel to be removed/repositioned, which is conducive for the fault-tolerant adhesion of the hydrogel adhesives during surgery. Besides, the hydrogels present good biocompatibility, near-infrared-assisted photothermal antibacterial activity, antioxidation and repeated thermo-responsive reversible adhesion and good hemostatic effect. The in vivo incision closure evaluation demonstrated their capability to promote the post-wound-closure and wound healing of the incisions, indicating that the developed reversible adhesive hydrogel dressing could serve as versatile tissue sealant.

          Supplementary Information

          The online version contains supplementary material available at 10.1007/s40820-022-00928-z.

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          Most cited references71

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          Mussel-inspired surface chemistry for multifunctional coatings.

          We report a method to form multifunctional polymer coatings through simple dip-coating of objects in an aqueous solution of dopamine. Inspired by the composition of adhesive proteins in mussels, we used dopamine self-polymerization to form thin, surface-adherent polydopamine films onto a wide range of inorganic and organic materials, including noble metals, oxides, polymers, semiconductors, and ceramics. Secondary reactions can be used to create a variety of ad-layers, including self-assembled monolayers through deposition of long-chain molecular building blocks, metal films by electroless metallization, and bioinert and bioactive surfaces via grafting of macromolecules.
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            Functional Hydrogels as Wound Dressing to Enhance Wound Healing

            Hydrogels, due to their excellent biochemical and mechnical property, have shown attractive advantages in the field of wound dressings. However, a comprehensive review of the functional hydrogel as a wound dressing is still lacking. This work first summarizes the skin wound healing process and relates evaluation parameters and then reviews the advanced functions of hydrogel dressings such as antimicrobial property, adhesion and hemostasis, anti-inflammatory and anti-oxidation, substance delivery, self-healing, stimulus response, conductivity, and the recently emerged wound monitoring feature, and the strategies adopted to achieve these functions are all classified and discussed. Furthermore, applications of hydrogel wound dressing for the treatment of different types of wounds such as incisional wound and the excisional wound are summarized. Chronic wounds are also mentioned, and the focus of attention on infected wounds, burn wounds, and diabetic wounds is discussed. Finally, the future directions of hydrogel wound dressings for wound healing are further proposed.
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              Tough adhesives for diverse wet surfaces

              Adhesion to wet and dynamic surfaces, including biological tissues, is important in many fields, but has proven extremely challenging. Existing adhesives are either cytotoxic, adhere weakly to tissues, or cannot be utilized in wet environments. We report a bio-inspired design for adhesives consisting of two layers: an adhesive surface and a dissipative matrix. The former adheres to the substrate by electrostatic interactions, covalent bonds, and physical interpenetration. The latter amplifies energy dissipation through hysteresis. The two layers synergistically lead to higher adhesion energy on wet surfaces than existing adhesives. Adhesion occurs within minutes, independent of blood exposure, and compatible with in vivo dynamic movements. This family of adhesives may be useful in many areas of application, including tissue adhesives, wound dressings and tissue repair.
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                Author and article information

                Contributors
                baoling@mail.xjtu.edu.cn
                Journal
                Nanomicro Lett
                Nanomicro Lett
                Nano-Micro Letters
                Springer Nature Singapore (Singapore )
                2311-6706
                2150-5551
                13 September 2022
                13 September 2022
                December 2022
                : 14
                : 185
                Affiliations
                [1 ]GRID grid.43169.39, ISNI 0000 0001 0599 1243, State Key Laboratory for Mechanical Behavior of Materials, and Frontier Institute of Science and Technology, , Xi’an Jiaotong University, ; Xi’an, 710049 People’s Republic of China
                [2 ]GRID grid.43169.39, ISNI 0000 0001 0599 1243, Key Laboratory of Shaanxi Province for Craniofacial Precision Medicine Research, College of Stomatology, , Xi’an Jiaotong University, ; Xi’an, 710049 People’s Republic of China
                Article
                928
                10.1007/s40820-022-00928-z
                9470803
                36098823
                999a7aaf-2436-4b69-8cde-70cfcff45849
                © The Author(s) 2022

                Open AccessThis article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article's Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article's Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.

                History
                : 16 June 2022
                : 29 July 2022
                Funding
                Funded by: Shanghai Jiao Tong University
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                Article
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                © The Author(s) 2022

                bioinspired injectable hydrogel,tissue sealant,temperature-dependent adhesion,reversible adhesion,wound healing

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