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      Robust and dynamic underwater adhesives enabled by catechol-functionalized poly(disulfides) network

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          ABSTRACT

          Developing molecular approaches to the creation of robust and water-resistant adhesive materials promotes a fundamental understanding of interfacial adhesion mechanisms as well as future applications of biomedical adhesive materials. Here, we present a simple and robust strategy that combines natural thioctic acid and mussel-inspired iron-catechol complexes to enable ultra-strong adhesive materials that can be used underwater and simultaneously exhibit unprecedentedly high adhesion strength on diverse surfaces. Our experimental results show that the robust crosslinking interaction of the iron-catechol complexes, as well as high-density hydrogen bonding, are responsible for the ultra-high interfacial adhesion strength. The embedding effect of the hydrophobic solvent-free network of poly(disulfides) further enhances the water-resistance. The dynamic covalent poly(disulfides) network also makes the resulting materials reconfigurable, thus enabling reusability via repeated heating and cooling. This molecule-engineering strategy offers a general and versatile solution to the design and construction of dynamic supramolecular adhesive materials.

          Abstract

          A robust underwater adhesive material is achieved by coupling natural thioctic acid with mussel-inspired iron-catechol chemistry, showing a high-strength, tunable and reusable adhesion to diverse surfaces.

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          25th anniversary article: The evolution of electronic skin (e-skin): a brief history, design considerations, and recent progress.

          Human skin is a remarkable organ. It consists of an integrated, stretchable network of sensors that relay information about tactile and thermal stimuli to the brain, allowing us to maneuver within our environment safely and effectively. Interest in large-area networks of electronic devices inspired by human skin is motivated by the promise of creating autonomous intelligent robots and biomimetic prosthetics, among other applications. The development of electronic networks comprised of flexible, stretchable, and robust devices that are compatible with large-area implementation and integrated with multiple functionalities is a testament to the progress in developing an electronic skin (e-skin) akin to human skin. E-skins are already capable of providing augmented performance over their organic counterpart, both in superior spatial resolution and thermal sensitivity. They could be further improved through the incorporation of additional functionalities (e.g., chemical and biological sensing) and desired properties (e.g., biodegradability and self-powering). Continued rapid progress in this area is promising for the development of a fully integrated e-skin in the near future. © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
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            Plant-inspired adhesive and tough hydrogel based on Ag-Lignin nanoparticles-triggered dynamic redox catechol chemistry

            Adhesive hydrogels have gained popularity in biomedical applications, however, traditional adhesive hydrogels often exhibit short-term adhesiveness, poor mechanical properties and lack of antibacterial ability. Here, a plant-inspired adhesive hydrogel has been developed based on Ag-Lignin nanoparticles (NPs)triggered dynamic redox catechol chemistry. Ag-Lignin NPs construct the dynamic catechol redox system, which creates long-lasting reductive-oxidative environment inner hydrogel networks. This redox system, generating catechol groups continuously, endows the hydrogel with long-term and repeatable adhesiveness. Furthermore, Ag-Lignin NPs generate free radicals and trigger self-gelation of the hydrogel under ambient environment. This hydrogel presents high toughness for the existence of covalent and non-covalent interaction in the hydrogel networks. The hydrogel also possesses good cell affinity and high antibacterial activity due to the catechol groups and bactericidal ability of Ag-Lignin NPs. This study proposes a strategy to design tough and adhesive hydrogels based on dynamic plant catechol chemistry.
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              Mechanically robust, readily repairable polymers via tailored noncovalent cross-linking

              Expanding the range of healable materials is an important challenge for sustainable societies. Noncrystalline, high molecular weight polymers generally form mechanically robust materials, which, however, are difficult to repair once they are fractured. This is because their polymer chains are heavily entangled and diffuse too sluggishly to unite fractured surfaces within reasonable timescales. Here, we report that low molecular weight polymers, when cross-linked by dense hydrogen bonds, give mechanically robust yet readily repairable materials, despite their extremely slow diffusion dynamics. A key was to utilize thiourea, which anomalously forms a zigzag hydrogen-bonded array that does not induce unfavorable crystallization. Another key was to incorporate a structural element for activating the exchange of hydrogen-bonded pairs, which enables the fractured portions to rejoin readily upon compression.
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                Author and article information

                Contributors
                Journal
                Natl Sci Rev
                Natl Sci Rev
                nsr
                National Science Review
                Oxford University Press
                2095-5138
                2053-714X
                February 2023
                25 July 2022
                25 July 2022
                : 10
                : 2
                : nwac139
                Affiliations
                Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, School of Chemistry and Molecular Engineering, East China University of Science and Technology , Shanghai 200237, China
                Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, School of Chemistry and Molecular Engineering, East China University of Science and Technology , Shanghai 200237, China
                Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, School of Chemistry and Molecular Engineering, East China University of Science and Technology , Shanghai 200237, China
                Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, School of Chemistry and Molecular Engineering, East China University of Science and Technology , Shanghai 200237, China
                Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, School of Chemistry and Molecular Engineering, East China University of Science and Technology , Shanghai 200237, China
                Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, School of Chemistry and Molecular Engineering, East China University of Science and Technology , Shanghai 200237, China
                Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, School of Chemistry and Molecular Engineering, East China University of Science and Technology , Shanghai 200237, China
                Author notes
                Corresponding author. E-mail: dahui_qu@ 123456ecust.edu.cn
                Author information
                https://orcid.org/0000-0002-2039-3564
                Article
                nwac139
                10.1093/nsr/nwac139
                10042223
                36994382
                8b070ff2-b4cc-4c2b-9f04-b1ed367cd4f8
                © The Author(s) 2022. Published by Oxford University Press on behalf of China Science Publishing & Media Ltd.

                This is an Open Access article distributed under the terms of the Creative Commons Attribution License ( https://creativecommons.org/licenses/by/4.0/), which permits unrestricted reuse, distribution, and reproduction in any medium, provided the original work is properly cited.

                History
                : 07 July 2021
                : 10 October 2021
                : 15 February 2022
                : 27 March 2023
                Page count
                Pages: 9
                Funding
                Funded by: National Natural Science Foundation of China, DOI 10.13039/501100001809;
                Award ID: 22025503
                Award ID: 21790361
                Award ID: 21871084
                Award ID: 21672060
                Funded by: Shanghai Municipal Science and Technology Commission, DOI 10.13039/501100003399;
                Award ID: 2018SHZDZX03
                Award ID: 17520750100
                Funded by: Fundamental Research Funds for the Central Universities, DOI 10.13039/501100012226;
                Funded by: Program of Introducing Talents of Discipline to Universities, DOI 10.13039/501100012176;
                Award ID: B16017
                Funded by: Program of Shanghai Academic/Technology Research Leader, DOI 10.13039/501100012247;
                Award ID: 19XD1421100
                Funded by: Institute for Advanced Study, DOI 10.13039/100005235;
                Award ID: SN-ZJU-SIAS-006
                Categories
                Research Article
                Chemistry
                AcademicSubjects/MED00010
                AcademicSubjects/SCI00010
                Nsr/1

                adhesives,supramolecular materials,dynamic polymers,non-covalent crosslink,iron-catechol complexes

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