Department of Chemical Engineering, Pohang University of Science and Technology, Pohang 37673, Republic of Korea.
Department of Chemistry, Institute for Molecular Science and Fusion Technology, Kangwon Radiation Convergence Research Support Center, Kangwon National University, Chuncheon 24341, Republic of Korea.
Biomacromolecules. 2024 Jan 8;25(1):379-387. doi: 10.1021/acs.biomac.3c01025. Epub 2023 Dec 18.
Mussels are marine organisms that are capable of constructing an underwater adhesion between their bodies and rigid structures. It is well known that mussels achieve underwater adhesion through the presence of mussel adhesive proteins (MAPs) that contain high levels of 3,4-dihydroxyphenylalanine (DOPA). Although the extraordinary underwater adhesive properties of mussels are attributed to DOPA, its capacity to play a dual role in surface adhesion and internal cohesion is inherently limited. However, mussels employ a combination of chemical moieties, not just DOPA, along with anatomical components, such as plaque and byssus, in underwater adhesion. This also involves junction proteins that connect the plaque and byssus. In this study, a novel hybrid MAP was bioengineered via the fusion of the plaque protein (foot protein type 1) and the histidine-rich domain of the junction protein (foot protein type 4). To achieve direct adhesion underwater, the adhesive should maintain surface adhesion without disintegrating. Notably, the histidine-Zn-coordinated hybrid MAP hydrogel maintained a high surface adhesion ability even after cross-linking because of the preservation of its unoxidized and non-cross-linked DOPA moieties. The formulated adhesive hydrogel system based on the bioengineered hybrid MAP exhibited self-healing properties, owing to the reversible metal coordination bonds. The developed adhesive hydrogel exhibits outstanding levels of bulk adhesion in underwater environments, highlighting its potential as an effective adhesive biomaterial. Therefore, the introduction of histidine-rich domains into MAPs may be applied in various studies to formulate mussel-inspired adhesives with self-healing properties and to fully utilize the adhesive ability of DOPA.
贻贝是一种能够在其身体和刚性结构之间构建水下黏附的海洋生物。众所周知，贻贝通过存在富含 3,4-二羟基苯丙氨酸 (DOPA) 的贻贝黏附蛋白 (MAPs) 来实现水下黏附。尽管贻贝具有非凡的水下黏附特性归因于 DOPA，但它在表面黏附和内部内聚中发挥双重作用的能力本质上是有限的。然而，贻贝在水下黏附中采用了多种化学基团，而不仅仅是 DOPA，以及解剖结构，如斑块和贻贝丝。这还涉及连接斑块和贻贝丝的连接蛋白。在这项研究中，通过融合斑块蛋白（足蛋白 1 型）和连接蛋白的组氨酸丰富结构域，生物工程合成了一种新型混合 MAP。为了实现水下直接黏附，黏附物应保持表面黏附而不分解。值得注意的是，由于未氧化和未交联的 DOPA 部分得以保留，组氨酸-Zn 配位的混合 MAP 水凝胶即使交联后仍保持高表面黏附能力。基于生物工程混合 MAP 配方的黏附水凝胶系统具有自修复特性，这是由于可逆的金属配位键。开发的黏附水凝胶在水下环境中表现出出色的整体黏附能力，突出了其作为有效黏附生物材料的潜力。因此，将富含组氨酸的结构域引入 MAP 中可能会应用于各种研究中，以配制具有自修复特性的贻贝启发型黏附剂，并充分利用 DOPA 的黏附能力。
