A double crosslinking adhesion mechanism for developing tough hydrogel adhesives
A double crosslinking adhesion mechanism for developing tough hydrogel adhesives
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DOI：
10.1016/j.actbio.2022.07.028
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发表时间：
2022-08-31
影响因子：
9.7
通讯作者：
Wang, Hua
中科院分区：
文献类型：
--
作者：
Han, Joonsu;Park, Jihoon;Wang, Hua
A-B-S-T-R-A-C-T强韧水凝胶粘合剂具有良好的凝胶网络，能很好地粘合湿组织，是下一代生物粘合剂的发展方向。虽然可以利用各种化学方法来构建坚韧的凝胶网络，但用于组织黏附的共价偶联方法仍然有限。在这里，我们首次报道了使用无副产物的胺-硫代内酯化学，这种化学引发了双交联胶粘机理，以开发出坚韧的凝胶粘合剂。硫内酯基团可以通过开环反应与组织表面胺偶联。生成的硫醇端基可以进一步交联成二硫键，从而能够形成坚固而稳定的粘附层。由甲基丙烯酸改性明胶、丙烯酸和硫代内酯丙烯酰胺组成的含硫代内酯的增韧水凝胶具有良好的生物相容性和力学性能，与各种工程固体和组织具有很强的粘附性。我们还展示了它作为组织密封剂和药库的能力。这种新的黏附机制将使未来用于止血、药物输送、组织修复和其他应用的生物黏附剂的设计多样化。重要声明坚韧水凝胶粘合剂具有优异的组织粘附性和机械性能，在止血、组织修复和药物输送应用方面显示出巨大的前景。然而，组织黏附的共价化学已经受到限制，这使得设计生物黏附剂的材料选择变窄，并可能造成安全问题。在这里，我们第一次报告了使用无副产物的胺-硫代内酯化学，它涉及到双交联性粘合机理，用于开发坚韧的水凝胶粘合剂。我们证明了含硫内酯的韧性水凝胶具有良好的生物相容性和力学性能，以及对工程固体和组织的良好粘附性。我们的新粘合技术将极大地促进未来用于众多生物医学应用的先进生物粘合剂的发展。(C)2022 Acta Materialia Inc.由爱思唯尔有限公司出版。保留所有权利。
A B S T R A C T Tough hydrogel adhesives that consist of a robust gel network and can strongly adhere to wet tissues have shown great promise as the next generation of bioadhesives. While a variety of chemistries can be utilized to construct the tough gel network, the covalent conjugation methods for tissue adhesion are still limited. Here we report, for the first time, the use of side product-free amine-thiolactone chemistry which initiates a double crosslinking adhesion mechanism to develop tough gel adhesives. Thiolactone groups can conjugate with tissue-surface amines via a ring-opening reaction. The resultant thiol end groups can be further crosslinked into disulfide linkages, enabling the formation of a robust and stable adhesion layer. The thiolactone-bearing tough hydrogel composed of methacrylate-modified gelatin, acrylic acid, and thiolacone acrylamide exhibited good biocompatibility and mechanical properties, and strong adhe-sion to various types of engineering solids and tissues. We also demonstrated its ability to function as a tissue sealant and drug depot. The novel adhesion mechanism will diversify future design of bioadhesives for hemostasis, drug delivery, tissue repair, and other applications. Statement of significance Tough hydrogel adhesives with excellent tissue-adhesive and mechanical properties have demonstrated tremendous promise for hemostasis, tissue repair, and drug delivery applications. However, the covalent chemistry for tissue adhesion has been limited, which narrows the choice of materials for the design of bioadhesives and may pose a safety concern. Here, for the first time, we report the use of side product -free amine-thiolactone chemistry, which involves a double crosslinking adhesion mechanism, for develop-ing tough hydrogel adhesives. We demonstrate that thiolactone-bearing tough hydrogels exhibit favorable biocompatibility and mechanical properties, and superior adhesion to both engineering solids and tis-sues. Our new adhesion technology will greatly facilitate future development of advanced bioadhesives for numerous biomedical applications. (c) 2022 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.