Design and Preparation of Antifreeze Silk-based Bioadhesive

Xin-yang Li; Ni Chen; Gong-wen Yang; Zheng-zhong Shao

doi:10.11777/j.issn1000-3304.2024.24104

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Design and Preparation of Antifreeze Silk-based Bioadhesive

Research Article | 更新时间：2024-12-24

- Design and Preparation of Antifreeze Silk-based Bioadhesive
- Acta Polymerica Sinica Vol. 55, Issue 11, Pages: 1463-1475(2024)
- 作者机构：
  
  聚合物分子工程国家重点实验室复旦大学先进材料实验室高分子科学系上海 200433
- 作者简介：
  
  Zheng-zhong Shao, E-mail: zzshao@fudan.edu.cn
- 基金信息：
- DOI：10.11777/j.issn1000-3304.2024.24104
  CLC：
- CSTR：32057.14.GFZXB.2024.7259
- Received：07 April 2024，
  
  Accepted：2024-05-11，
  
  Published Online：21 August 2024，
  
  Published：20 November 2024
- 稿件说明：
移动端阅览
李欣阳, 陈旎, 杨公雯, 邵正中. 抗冻型丝蛋白胶黏剂的设计与制备. 高分子学报, 2024, 55(11), 1463-1475

Li, X. Y.; Chen, N.; Yang, G. W.; Shao, Z. Z. Design and preparation of antifreeze silk-based bioadhesive. Acta Polymerica Sinica, 2024, 55(11), 1463-1475
李欣阳, 陈旎, 杨公雯, 邵正中. 抗冻型丝蛋白胶黏剂的设计与制备. 高分子学报, 2024, 55(11), 1463-1475 DOI： 10.11777/j.issn1000-3304.2024.24104. CSTR： 32057.14.GFZXB.2024.7259.

Li, X. Y.; Chen, N.; Yang, G. W.; Shao, Z. Z. Design and preparation of antifreeze silk-based bioadhesive. Acta Polymerica Sinica, 2024, 55(11), 1463-1475 DOI： 10.11777/j.issn1000-3304.2024.24104. CSTR： 32057.14.GFZXB.2024.7259.

摘要

为应对传统化学黏合剂因环境污染和潜在健康风险所带来的挑战，本研究在成功制备一款天然桑蚕丝蛋白和单宁酸复合胶黏剂的同时，很好地解决了传统黏合剂在低温环境下无法工作或性能不佳等问题. 通过在丝蛋白中引入与其有强相互作用的单宁酸，抑制了丝蛋白由无规卷曲构象向

-折叠构象的转变，进而保障了此复合胶黏剂的强黏附力. 在优化丝蛋白与单宁酸复合物配比的基础上，选用乙二醇和水二元溶剂体系，不仅有效提升了此生物基胶黏剂溶解性能和对各种基体黏结的普适性，并且显著降低了其冻结点，赋予了其相应的抗冻性能. 实验结果证实，此生物基胶黏剂在从-20 ℃到室温范围内均展现出超越传统商用化学黏合剂和其他生物基黏合剂的黏附能力. 因此，所研发的抗冻型丝蛋白生物基胶黏剂，以其环保性、生物降解性及在低温条件下出色的黏结性能，在包装、生物医疗及环境保护等领域中具有很好的应用前景.

Abstract

Amidst growing demands for environmental protection and sustainable development

there is an urgent need within the industry for alternatives to traditional chemical adhesives

which are implicated in environmental contamination and health hazards. This study introduces an antifreeze silk fibroin bioadhesive designed to address the performance deficits of conventional bio-based adhesives in frozen conditions. The synthesis of this novel silk-derived adhesive employs a dual-stage process: initially crafting a silk fibroin-based adhesive matrix

followed by its integ

ration with an aqueous solvent system to formulate the bioadhesive. This approach enables the long-term storage of protein powders under ambient conditions

with the flexibility of formulation and application upon demand. Additionally

the adhesive strength is readily adjustable through the modulation of substrate concentration. The adhesive efficacy is principally reliant on the hydrogen bonding capability

with the quantity of hydrogen bond sites provided by silk fibroin critically influencing the protein adhesive's binding properties. Incorporation of tannic acid

known for its strong affinity with silk fibroin

prevents the transition of silk fibroin chains from a random coil to a

β‍

-sheet

thereby preserving the bioadhesive's strength. The study further refines the silk fibroin to tannic acid ratio and solvent composition

opting for a binary solvent system of ethylene glycol and water. This choice markedly enhances the solubility of the silk fibroin bioadhesive and significantly depresses its freezing point

augmenting its antifreeze capabilities and facilitating substrate bonding at low temperatures. The adhesive also exhibits exceptional low-temperature stability and adaptability to fluctuations in ambient temperature. Experimental validations demonstrate that this bioadhesive surpasses the adhesive performance of conventional commercial chemical adhesives and other bio-based adhesives over a broad temperature range from -24 °C to room temperature. Consequently

the antifreeze silk fibroin bioadhesive developed in this study

with its eco-friendliness

biodegradability

and exceptional adhesive performance under extreme low-temperature conditions

shows great potential for applications in key areas such as packaging

biomedical

and environmental protection.

关键词

Keywords

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