Regenerated Silk Fibroin Hydrogel with Laponite/Polydopamine Composite Nanoparticles

Gao-huan Da; Yi-qun Ma; Qin-rui Lin; Zheng-zhong Shao

doi:10.11777/j.issn1000-3304.2022.22190

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Regenerated Silk Fibroin Hydrogel with Laponite/Polydopamine Composite Nanoparticles

Research Article | 更新时间：2023-05-22

- Regenerated Silk Fibroin Hydrogel with Laponite/Polydopamine Composite Nanoparticles
  增强出版
- ACTA POLYMERICA SINICA Vol. 54, Issue 1, Pages: 95-105(2023)
- 作者机构：
  
  1.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
  2.复旦大学附属中山医院上海 200032
- 作者简介：
  
  Zheng-zhong Shao, E-mail: zzshao@fudan.edu.cn
- 基金信息：
- DOI：10.11777/j.issn1000-3304.2022.22190
  CLC：
- Published：20 January 2023，
  
  Published Online：28 September 2022，
  
  Received：19 May 2022，
  
  Accepted：20 June 2022
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达高欢,马易群,林沁睿等.含有锂皂土/聚多巴胺复合纳米微粒的再生丝蛋白水凝胶[J].高分子学报,2023,54(01):95-105.

Da Gao-huan,Ma Yi-qun,Lin Qin-rui,et al.Regenerated Silk Fibroin Hydrogel with Laponite/Polydopamine Composite Nanoparticles[J].ACTA POLYMERICA SINICA,2023,54(01):95-105.
达高欢,马易群,林沁睿等.含有锂皂土/聚多巴胺复合纳米微粒的再生丝蛋白水凝胶[J].高分子学报,2023,54(01):95-105. DOI： 10.11777/j.issn1000-3304.2022.22190.

Da Gao-huan,Ma Yi-qun,Lin Qin-rui,et al.Regenerated Silk Fibroin Hydrogel with Laponite/Polydopamine Composite Nanoparticles[J].ACTA POLYMERICA SINICA,2023,54(01):95-105. DOI： 10.11777/j.issn1000-3304.2022.22190.

摘要

在辣根过氧化物酶/过氧化氢酶促交联(化学交联)制备再生丝蛋白化学交联凝胶的过程中，通过引入锂皂土/聚多巴胺复合纳米材料作为第二组分，以调节反应并提高化学交联效率；再经乙醇熟化后，再生丝蛋白化学交联凝胶中可进一步形成物理网络，进而得到双交联凝胶. 结果表明，第二组分的引入不仅能够提高再生丝蛋白化学交联水凝胶的力学性能，并有利于后续均匀物理交联网络的形成，致使最终所得双交联水凝胶具有更好的力学性能. 同时，由此制备的双交联水凝胶传承了再生丝蛋白良好的生物相容性以及与交联结构密切相关的生物降解性，并具备了诱导干细胞成骨分化的能力，因而在软骨修复等领域具有潜在的应用价值.

Abstract

Regenerated silk fibroin (RSF) hydrogel has been widely used in the field of tissue engineering due to its good biocompatibility

degradability and low immunogenicity. It shows a good application prospect in the field of cartilage repair. However

as a natural polymer hydrogel

the strength of RSF hydrogel is difficult to match with cartilage. In this study

during the preparation of RSF chemical crosslinked hydrogel by horseradish peroxidase (HRP)/hydrogen peroxide (H

) enzymatic crosslinking

laponite (LAP)/polydopamine (PDA) composite nanomaterials were introduced as a second component to adjust the reaction and improve the chemical crosslinking efficiency. Compared with the pure RSF chemically crosslinked hydrogel

the mechanical properties of the composite hydrogel were significantly improved after the addition of LAP/PDA composite nanomaterials

and the compression modulus was improved by about 70%. This is mainly because the LAP/PDA composite nanomaterials inhibited the "curling" of silk protein molecular chains in the crosslinking process by participating in the enzymatic crosslinking reaction

and increased the chemical crosslinking points in the crosslinked network. After soaking in ethanol

physical crosslinked network can be further formed in RSF chemical crosslinked hydrogel to obtain a double crosslinked hydrogel. The increase of chemical crosslinking points in the RSF-LAP/PDA chemical crosslinked hydrogel was beneficial to decreasing the dimensions and improving the distribution uniformity of the

-sheet domains formed during ethanol ripening

such that the mechanical properties of the final double crosslinked hydrogel were greatly improved. This double crosslinked method can effectively solve the problem of mechanical properties degradation caused by inhomogeneous crosslinked network when preparing RSF hydrogel with high solid content

and improve the stability of regenerated silk fibroin based hydrogel as implant repair materials

in vivo

In vitro

study showed that the RSF-LAP/PDA double crosslinked hydrogel had excellent biocompatibility and the ability to induce osteogenic differentiation of stem cells

which made it good application prospect in cartilage repair and other fields.

关键词

丝蛋白水凝胶酶交联物理交联双交联

Keywords

Silk fibroinHydrogelEnzymatic crosslinkingPhysical crosslinkingDouble crosslinking

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