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化学进展 2021, Vol. 33 Issue (12): 2378-2391 DOI: 10.7536/PC201122 前一篇   后一篇

• 综述 •

基于贻贝启发的水下仿生胶黏剂

王桂龙1, 崔辛1, 陈莹1, 胡振峰1, 梁秀兵1,*(), 陈甫雪2,*()   

  1. 1 军事科学院国防科技创新研究院 北京 100071
    2 北京理工大学化学与化工学院 北京 100081
  • 收稿日期:2020-11-18 修回日期:2021-04-04 出版日期:2021-12-20 发布日期:2021-07-29
  • 通讯作者: 梁秀兵, 陈甫雪
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Underwater Biomimetic Adhesive Based on Mussel Inspiration

Guilong Wang1, Xin Cui1, Ying Chen1, Zhen-feng Hu1, Xiubing Liang1(), Fuxue Chen2()   

  1. 1 Defense Innovation Institute, Academy of Military Science,Beijing 100071, China
    2 School of Chemistry & Chemical Engineering, Beijing Institute of Technology,Beijing 100081, China
  • Received:2020-11-18 Revised:2021-04-04 Online:2021-12-20 Published:2021-07-29
  • Contact: Xiubing Liang, Fuxue Chen

海洋中的贻贝依靠丝足(Byssus)与足盘(Plaque)可以在潮湿及水下环境中快速而牢固地黏附于各种固体表面。贻贝强健的足部具有沟渠状的生理结构,通过类似于“注塑生产”的生理过程,它们可以生成丝足与足盘。贻贝将液态的蛋白质挤压到沟渠里,只需几秒钟时间,这些蛋白质就能形成一条条发丝一样纤细的丝足。每条丝足的末端都有一个黏性足盘,足盘可以牢牢地黏附在岩石及固体表面。丝足及足盘由多种黏附蛋白(Mfps)组成,且几乎每种黏附蛋白都含有L-3,4-二羟基苯丙氨酸(DOPA)成分。在过去的数十年间,科研人员基本揭示了贻贝黏附蛋白的结构及其黏附机理。DOPA的儿茶酚基团,通过氧化交联、金属螯合、氢键、静电作用、疏水作用、π-π作用、阳离子-π作用等各种共价和非共价相互作用,实现强大的界面黏接。基于贻贝黏附蛋白的结构及其黏附机理,通过使用DOPA及其类似物修饰的聚合物体系,人们得到了多种具有优秀机械性能和功能化的新型仿生多巴类水下胶黏剂。本综述首先介绍了贻贝黏附蛋白的组成特点及其黏附机理;随后分别介绍了凝聚层类胶黏剂、水凝胶类胶黏剂、智能型水下胶黏剂的结构特点及黏附机理;最后讨论了目前仿生水下胶黏剂存在的问题及未来发展前景。

关键词： 贻贝, 水下胶黏剂, 仿生材料, 儿茶酚

Marine mussels can quickly and firmly anchor to foreign surfaces in seawater using their byssus and plaque. Mussels produce byssus and plaque through a physiological process similar to “injection production”. Mussels squeeze liquid protein into the ventral groove on their feet, which will then form hair-like byssus in seconds. Each byssus connects with a plaque at its end, and the plaque can firmly adhere to rocks or other solid surfaces. Byssus and plaque are composed of a variety of mussel foot proteins (Mfps), and almost every Mfps contains L-3,4-dihydroxyphenylalanine (DOPA). In the past few decades, researchers have basically revealed the structure of Mfps and their adhesion mechanism. The catechol group of DOPA achieves strong interfacial bonding through a variety of covalent and non-covalent interactions, such as oxidative crosslinking, metal-catechol coordination, hydrogen bonding, electrostatic interaction, hydrophobic interactions, π-π interactions, cation-π interactions, etc. Based on the structure of Mfps and their adhesion mechanism, a variety of new biomimetic DOPA adhesives with excellent mechanical properties and functionalization have been obtained using polymer system modified by DOPA and its analogues. In this review, we first introduce the composition and adhesion mechanism of Mfps, then discuss the corresponding structure characteristics and adhesion mechanism of coacervate adhesives, hydrogels adhesives and intelligent adhesives. Finally, the existing problems and future development prospects of underwater biomimetic adhesives are presented.

Contents

1 Introduction

2 Species and distribution of mussel foot proteins

3 Adhesion mechanism of mussel foot proteins

4 Research progress of underwater biomimetic adhesives

4.1 Coacervate type of underwater adhesives

4.2 Hydrogel type of underwater adhesive

4.3 Smart type of underwater adhesive

4.4 DOPA-free type of underwater adhesives

5 Application prospect of underwater adhesives

5.1 Anti-corrosion and maintenance of ships

5.2 Surgical wound suturing and tissue repair

5.3 Intelligent biomimetic equipment

6 Conclusion and outlook

Key words: mussel, underwater adhesive, biomimetic materials, catechol
()
图1 贻贝依靠丝足和足盘黏附在固体表面[5]
Fig.1 Mussels anchor to foreign surfaces by means of byssus and plaque[5]
表1 贻贝黏附蛋白的结构特点及分布位置[5,19⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓~40]
Table 1 Composition characteristics and localization of mussel foot proteins[5,19⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓~40]
Mussel foot proteins Mass (kDa) PI DOPA (mol %) Location References
Mfp-1 90~110 10.5 15 surface of plaque 19~23
Mfp-2 45 9.5 5 in the plaque 24~28
Mfp-3F 5~7 9 7~20 at interface of the plaque 30
Mfp-3S 5~7 9 8~14 at interface of the plaque 30~32
Mfp-4 93 9.5 4 in the plaque 34
Mfp-5 10 9 30 at interface of the plaque 35~39
Mfp-6 11.6 9.5 3 at interface of the plaque 40
图2 (a)邻苯二酚基团参与形成内聚力机理[28], (b)邻苯二酚基团在各种固体表面黏附机理[26]
Fig.2 (a) Catechol groups are involved in the formation of cohesion mechanism[28], (b) The adhesion mechanism of catechol groups on various solid surfaces[26]
图3 阳离子对儿茶酚类胶黏剂的影响。(a)同时含有赖氨酸和儿茶酚结构;(b)同时含有精氨酸和儿茶酚结构;(c)只含有儿茶酚结构;(d)只含有阳离子结构[56]
Fig.3 Chemical structures of catechol analogs that were used to investigate the influence of cations on the adhesive performance of catechol-containing tripeptides. (a) and (b) contain both catechols and cations; (c) only contains catechols, while (d) only contains cations[56]
图4 儿茶酚基团和有机阳离子协同作用导致水下黏附原理[57]
Fig.4 The synergistic action of catechol groups and organic cations leads to the principle of underwater adhesion[57]
图5 聚磷酸多巴胺胶黏剂的结构及水下黏接机理[71]
Fig.5 Structure and mechanism of dopamine polyphosphate adhesive[71]
图6 QCS/PAAcat胶黏剂的结构及水下黏接机理[72]
Fig.6 Structure and underwater adhension mechanism of QCS/PAAcat adhesive[72]
图7 (a) 同电荷凝聚层的形成原理[Rmfp-1(绿色)、MADQUAT(灰色)];(b) Rmfp-1与MADQUAT同电荷凝聚层的光学显微镜图(比例尺, 50 μm.);(c)同电荷凝聚层的分相效果(比例尺, 1 cm.)。[73]
Fig.7 (a) Schematic of like-charged complex coacervate formation [Rmfp-1 (green) and MADQUAT (gray)]; (b) Light microscopy image of microdroplets of Rmfp-1 and MADQUAT like-charged coacervate. (Scale bar, 50 μm.); (c) Bulk phase separation of the like-charged coacervate. (Scale bar, 1 cm.)[73]
图8 iCMBAs类水凝胶的结构及制备[78]
Fig.8 Structure and preparation of iCMBAs hydrogel[78]
图9 海藻酸-儿茶酚水凝胶的结构及其黏附机理[79]
Fig.9 Structure and adhesion mechanism of alginic acid-catechol hydrogel[79]
图10 DOPA-Fe3+明胶水凝胶的结构及其黏附机理[80]
Fig.10 Structure and adhesion mechanism of DOPA-Fe3+ gelatin hydrogel[80]
图11 PAA/PMD水凝胶的结构及其黏附机理[81]
Fig.11 The structure and adhesion mechanism of PAA/PMD hydrogel[81]
图12 HA/Pluronic水凝胶的结构及温度响应机理[84]
Fig.12 Structure and temperature response mechanism of HA/Pluronic hydrogel[84]
图13 儿茶酚-硼酸酯胶黏剂结构及其温度响应机理[85]
Fig.13 The structure and temperature response mechanism of catechol-borate adhesive[85]
图14 (a) Fe3O4-TRGA的示意图及实拍图片;(b) Fe3O4-TRGA的NIR响应黏附能力转换机制示意图;(c)透射电镜(TEM)图像显示掺杂Fe3O4 NPs (0.2 wt%)在TRGA中的分布[86]
Fig.14 (a) Schematic diagram and real photos of the Fe3O4-TRGA; (b) Schematic diagram showing NIR-responsive adhesion switching mechanism for the Fe3O4-TRGA;(c) Transmission electron microscope (TEM) image showing the distribution of doped Fe3O4 NPs (0.2 wt%) in the TRGA[86]
图15 (a) Chitosan-Catechol-pNIPAM水下胶黏剂制备示意图;(b) Chitosan-Catechol-pNIPAM胶黏剂的可逆热响应机制;(c) 20 ℃; (d) 40 ℃, Chitosan-Catechol-pNIPAM溶液状态(50 mg/mL) (20 ℃为流动状态,40 ℃为交联态)[87]
Fig.15 (a) A schematic illustration of the preparation of the Chitosan-Catechol-pNIPAM biomacromolecular wet adhesive; (b) The mechanism for the chain state of the Chitosan-Catechol-pNIPAM biomacromolecule induced by the reversible thermo-responsive conformational change of pNIPAM side chains on the chitosan backbone (below the LCST, Chitosan-Catechol-pNIPAM is a linear branched macromolecule; above the LCST, Chitosan-Catechol-pNIPAM is a crosslinked macromolecule);(c) 20 ℃; (d) 40 ℃. Optical photographs showing the solution states (50 mg/mL) of Chitosan-Catechol-pNIPAM (20 ℃ is the flow state and 40 ℃ is cross-linked).[87]
图16 anth-PEI胶黏剂受光、热刺激响应示意图[88]
Fig.16 anth-PEI adhesives stimulated by light and heat[88]
图17 基于LMWMs的超分子黏接材料[89]
Fig.17 Supramolecular adhesives based on LMWMs[89]
图18 基于PNIPAM的胶黏剂结构及其温度响应机理[92]
Fig.18 PNIPAM based adhesive and its temperature response mechanism[92]
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摘要

基于贻贝启发的水下仿生胶黏剂