Cooperative Multivalent Weak and Strong Interfacial Interactions Enhance the Adhesion of Mussel-Inspired Adhesives
Cooperative Multivalent Weak and Strong Interfacial Interactions Enhance the Adhesion of Mussel-Inspired Adhesives
复制标题
DOI：
10.1021/acs.macromol.1c00742
复制
发表时间：
2021-06
期刊：
影响因子：
5.5
通讯作者：
Amal Narayanan;Sukhmanjot Kaur;Nityanshu Kumar;M. Tsige;Abraham Joy;A. Dhinojwala
中科院分区：
文献类型：
--
作者：
Amal Narayanan;Sukhmanjot Kaur;Nityanshu Kumar;M. Tsige;Abraham Joy;A. Dhinojwala
受贻贝足丝对表面的强粘附力的启发，在聚合物结构中掺入 3,4-二羟基苯丙氨酸 (DOPA) 已成为提高聚合物粘附力的流行策略。有大量文献报道这种仿生方法可以提高聚合物的粘合性能。然而，基于多巴的粘附成功背后的机制仍然是一个谜，因为将界面粘附对化学变化的贡献解耦在实验上具有挑战性。在这里，我们设计了具有四种不同功能的受贻贝启发的弹性体，以测试芳香族和羟基在确定粘合性能方面的重要性。通过结合附着力测量、表面敏感光谱和分子动力学模拟，我们发现芳香族基团与蓝宝石表面羟基形成弱的多价酸碱相互作用。此外，与用苯丙氨酸（仅芳族）、丝氨酸（仅羟基）或酪氨酸（芳族和一个羟基）基团功能化的聚合物类似物相比，DOPA 的苯基（弱酸碱相互作用）和 -OH 基团（强酸碱相互作用）与蓝宝石 -OH 基团的相互作用增加了基于 DOPA 的聚合物的粘附力。因此，这项研究说明了强酸碱相互作用和弱酸碱相互作用在增强粘附力方面的重要性。
Inspired by the strong adhesion of mussel byssal threads to surfaces, the incorporation of 3,4-dihydroxyphenylalanine (DOPA) in polymer architecture has become a popular strategy to improve the adhesion of the polymers. There are numerous literature reports of this bioinspired method to improve the adhesion performance of polymers. However, the mechanism behind the success of DOPA-based adhesion continues to be a puzzle as decoupling the contribution of interfacial adhesion to the alteration in chemistry is experimentally challenging. Herein, we designed mussel-inspired elastomers with four different functionalities to test the importance of aromatic and hydroxyl groups in determining the adhesion performance. With a combination of adhesion measurements, surface-sensitive spectroscopy, and molecular dynamics simulations, we show that the aromatic groups form weak multivalent acid–base interactions with the surface hydroxyl groups on sapphire. Also, the interaction of both phenyl (weak acid–base interaction) and −OH groups (strong acid–base interaction) of DOPA with sapphire −OH groups increases the adhesion of DOPA-based polymers compared to polymer analogs functionalized with either phenylalanine (only aromatic), serine (only hydroxyl), or tyrosine (aromatic and one hydroxyl) groups. Thus, this study illustrates the importance of both strong and weak acid–base interactions in enhancing adhesion.