Mussel-Inspired Self-Healing Double-Cross-Linked Hydrogels by Controlled Combination of Metal Coordination and Covalent Cross-Linking,Biomacromolecules

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Mussel-Inspired Self-Healing Double-Cross-Linked Hydrogels by Controlled Combination of Metal Coordination and Covalent Cross-Linking
Biomacromolecules ( IF 5.5 ) Pub Date : 2017-12-04 00:00:00 , DOI: 10.1021/acs.biomac.7b01249
Amanda Andersen ₁ , Marie Krogsgaard ₁ , Henrik Birkedal ₁

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Mussel-inspired hydrogels held together by reversible catecholato–metal coordination bonds have recently drawn great attention owing to their attractive self-healing, viscoelastic and adhesive properties together with their pH-responsive nature. A major challenge in these systems is to orchestrate the degree of catechol oxidation that occurs under alkaline conditions in air and has a great impact on the aforementioned properties because it introduces irreversible covalent cross-links to the system, which stiffens the hydrogels but consume catechols needed for self-healing. Herein, we present a catechol-based hydrogel design that allows for the degree of oxidative covalent cross-linking to be controlled. Double cross-linked hydrogels with tunable stiffness are constructed by adding the oxidizable catechol analogue, tannic acid, to an oxidation-resistant hydrogel construct held together by coordination of the dihydroxy functionality of 1-(2′-carboxyethyl)-2-methyl-3-hydroxy-4-pyridinone to trivalent metal ions. By varying the amount of tannic acid, the hydrogel stiffness can be customized to a given application while retaining the self-healing capabilities of the hydrogel’s coordination chemical component.

中文翻译：

金属配位和共价交联的可控组合，启发了贻贝启发的自修复双交联水凝胶

通过可逆的邻苯二酚-金属配位键结合在一起的以贻贝为灵感的水凝胶，由于其具有吸引力的自愈性，粘弹性和粘合性以及其对pH的响应特性，最近受到了广泛的关注。这些系统的主要挑战是协调在空气中碱性条件下发生的邻苯二酚氧化程度，并且对上述特性产生重大影响，因为它会向系统引入不可逆的共价交联键，从而使水凝胶变硬，但会消耗所需的邻苯二酚自我修复。在本文中，我们提出了一种基于儿茶酚的水凝胶设计，该设计允许控制氧化共价交联的程度。通过添加可氧化的邻苯二酚类似物单宁酸，通过将1-（2'-羧乙基）-2-甲基-3-羟基-4-吡啶酮的二羟基官能团配位成三价金属离子而结合在一起的抗氧化水凝胶结构。通过改变单宁酸的量，可以在给定应用中定制水凝胶的硬度，同时保留水凝胶配位化学成分的自愈能力。

更新日期：2017-12-04

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