贻贝黏附蛋白启发的甲壳素纳米晶须增强湿态黏附水凝胶的研究

梁子毅; 黄鸿键; 倪鹏; 徐仁凤; 王正朝; 刘海清

doi:10.11777/j.issn1000-3304.2022.22254

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贻贝黏附蛋白启发的甲壳素纳米晶须增强湿态黏附水凝胶的研究

研究论文 | 更新时间：2023-11-27

- 贻贝黏附蛋白启发的甲壳素纳米晶须增强湿态黏附水凝胶的研究
  增强出版
- Mussel Adhesive Protein Inspired Chitin Nanowiskers Enhanced Adhesive Hydrogels for Wet Adhesion
- 高分子学报 2023年54卷第3期页码：365-380
- 作者机构：
  
  1.福建师范大学，化学与材料学院，福州 350007
  2.福建师范大学，福建省高分子材料重点实验室，福州 350007
  3.福建师范大学，生命科学学院，福州 350007
- 作者简介：
  
  E-mail: haiqingliu@fjnu.edu.cn
- 基金信息：
  
  国家自然科学基金(基金号 ┣52103108);22175037┫;福建省工信厅教育厅联合重点项目(项目号 [2021]415-2021G02005)和福建省科技厅社会发展引导性项目(2020Y0020)
- DOI：10.11777/j.issn1000-3304.2022.22254
  中图分类号：
- 纸质出版日期：2023-03-20，
  
  网络出版日期：2022-10-17，
  
  收稿日期：2022-07-27，
  
  录用日期：2022-09-09
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梁子毅,黄鸿键,倪鹏等.贻贝黏附蛋白启发的甲壳素纳米晶须增强湿态黏附水凝胶的研究[J].高分子学报,2023,54(03):365-380.

Liang Zi-yi,Huang Hong-jian,Ni Peng,et al.Mussel Adhesive Protein Inspired Chitin Nanowiskers Enhanced Adhesive Hydrogels for Wet Adhesion[J].ACTA POLYMERICA SINICA,2023,54(03):365-380.
梁子毅,黄鸿键,倪鹏等.贻贝黏附蛋白启发的甲壳素纳米晶须增强湿态黏附水凝胶的研究[J].高分子学报,2023,54(03):365-380. DOI： 10.11777/j.issn1000-3304.2022.22254.

Liang Zi-yi,Huang Hong-jian,Ni Peng,et al.Mussel Adhesive Protein Inspired Chitin Nanowiskers Enhanced Adhesive Hydrogels for Wet Adhesion[J].ACTA POLYMERICA SINICA,2023,54(03):365-380. DOI： 10.11777/j.issn1000-3304.2022.22254.

摘要

报道了一种力学性能优良，湿态生物组织黏附能高的黏附水凝胶. 该凝胶由丙烯酸、甲基丙烯酸羟乙酯和3-三烯十五烷基-1

2-邻苯二酚共聚，与壳聚糖复合、并由甲壳素纳米晶须增强而成. 该凝胶网络含有可逆和不可逆交联作用. 其中可逆物理作用包括阴阳离子聚电解质静电吸引、烷基链疏水缔合、苯环

堆积、阳离子-

、氢键和拓扑纠缠. 由这些物理键形成的次级网络的可逆形成/破坏为水凝胶形变提供了能量耗散，从而提升了其断裂韧性. 另一方面，水凝胶的快速吸水能力破坏了湿润基体表面的水合层，使凝胶表面基团能与组织表面形成物理键和化学键的界面相互作用，从而共同促进水凝胶与湿态组织的强韧黏附. 水凝胶的断裂强度可达276.4 kPa，对湿润猪皮的界面黏附韧性可达831 J/m

，在水下对猪皮的界面黏附韧性约达236 J/m

，猪皮和猪肝伤口闭合强度分别可达26.2和16.5 kPa. 该黏附凝胶适合作为免缝合的伤口闭合黏胶材料.

Abstract

Aiming at the challenges of low mechanical adhesion and weak wet adhesion potential faced by the traditional adhesive hydrogels

a new design strategy for adhesive hydrogel is reported in this study. Inspired by the mussel adhesive protein and the synergistic effect between cations and catechols in wet adhesion

PAHU-CS-CNF hydrogel is synthesized

via

one-pot method copolymerizing acrylic acid (AA)

hydroxyethyl methacrylate (HEMA) and 3-trienopentadecyl-1

2-catechol (UH) with protonated chitosan (CS) and chitin nanowiskers (CNF) in aqueous solution. Since the reversible physical interactions include electrostatic attraction

hydrophobic association among alkyl chains

π‍

-‍

stacking of benzene rings

cation-‍

hydrogen bonding and topological entanglement

the secondary networks formed by these physical bonds provide good energy dissipation for the hydrogel deformation. The synergistic effects of cations

catechols

and the water absorbability of PAHU-CS-CNF hydrogel that destructs the hydration layer on the contact interface

enable the hydrogel to form solid interfacial physical and chemical bonds interactions with wet porcine skin surface. These unique structures and mechanisms of PAHU-CS-CNF hydrogel lead to good mechanical properties (fracture strength ~276.4 kPa

toughness ~633 kJ/m

)

excellent adhesion properties to porcine skin (interfacial toughness in wet state ~831 J/m

interfacial toughness underwater ~236 J/m

wound closure adhesion strength on skin ~26.2 kPa

wound closure adhesion strength on liver ~16.5 kPa)

and the hydrogel is not easy to adhere to skin tissue in the presence of serum

given potential to prevent the wound tissue from secondary damage. The hydrogel has a great selective adhesion on biological tissue over nonbiological substrates. The PAHU-CS-CNF adhesive hydrogel may be potentially applied in the field of sutureless wound closure.

关键词

贻贝黏附蛋白水凝胶湿态黏附黏附韧性

Keywords

Mussel adhesion proteinHydrogelWet state adhesionAdhesion toughness

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