基于双硫键交换可控构建的水凝胶及其动态交联机理研究

窦雪宇; 王星; 吴德成

doi:10.11777/j.issn1000-3304.2019.18263

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基于双硫键交换可控构建的水凝胶及其动态交联机理研究

专论 | 更新时间：2021-01-26

- 基于双硫键交换可控构建的水凝胶及其动态交联机理研究
- Study of Disulfide-exchange Dynamic Cross-linking Mechanism for Controlled Construction of Hydrogels
- 高分子学报 2019年50卷第5期页码：429-441
- 作者机构：
  
  1.中国科学院化学研究所北京分子科学国家研究中心　北京 100190
  2.中国科学院大学化学科学学院　北京 100049
- 作者简介：
  
  [ "吴德成，男，1975年出生. 1993 ~ 2001年就读于中国科学技术大学高分子科学与工程系，分别获得学士和硕士学位；2002 ~ 2006年就读于新加坡国立大学化学系，获得博士学位. 2005 ~ 2010年在新加坡材料与工程研究院从事研究工作，先后任研究工程师和高级研究工程师；2011年至今在中国科学院化学研究所工作，任研究员和课题组长；2015年起兼任中国科学院大学岗位教授. 2011年获中共中央组织部“青年千人”计划支持；2017年获国家自然科学基金杰出青年科学基金资助；2018年入选科技部中青年科技创新领军人才；2018年获教育部技术发明一等奖(排名第三). 目前研究方向为生物医用高分子的基础及应用研究，已发表SCI论文94篇，获PCT或美国发明专利授权6件，中国发明专利授权10件" ]
- 基金信息：
  
  国家自然科学基金(基金号 21725403，21674120)资助项目()
- DOI：10.11777/j.issn1000-3304.2019.18263
  中图分类号：
- 纸质出版日期：2019-5，
  
  网络出版日期：2019-2-26，
  
  收稿日期：2018-12-7，
  
  修回日期：2019-1-14，
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窦雪宇, 王星, 吴德成. 基于双硫键交换可控构建的水凝胶及其动态交联机理研究[J]. 高分子学报, 2019,50(5):429-441.

Xue-yu Dou, Xing Wang, De-cheng Wu. Study of Disulfide-exchange Dynamic Cross-linking Mechanism for Controlled Construction of Hydrogels[J]. Acta Polymerica Sinica, 2019,50(5):429-441.
窦雪宇, 王星, 吴德成. 基于双硫键交换可控构建的水凝胶及其动态交联机理研究[J]. 高分子学报, 2019,50(5):429-441. DOI： 10.11777/j.issn1000-3304.2019.18263.

Xue-yu Dou, Xing Wang, De-cheng Wu. Study of Disulfide-exchange Dynamic Cross-linking Mechanism for Controlled Construction of Hydrogels[J]. Acta Polymerica Sinica, 2019,50(5):429-441. DOI： 10.11777/j.issn1000-3304.2019.18263.

摘要

水凝胶是一种通过化学或物理作用交联形成的三维网络高分子材料. 近年来，采用动态共价键交联构建的智能水凝胶因其基础研究的重要性以及在生物医学领域中广泛的应用前景引起了众多科研工作者的关注，因而发展具有环境响应性或自修复特性的凝胶材料，能够满足其在生物医学领域中应用的更高要求. 本文结合国内外关于动态共价键制备刺激响应性凝胶的研究发展现状，系统地总结和评述了一种活性可控交联策略，能够通过控制外界响应刺激可逆地激活或终止“巯基-双硫键”交换反应，进而实现在宏观和微/纳米多尺度下凝胶结构和性能的可控构筑，为凝胶材料的多功能化构建提供了全新的思路，同时也为新型智能生物材料的设计和发展提供了一种普适化方法.

Abstract

Hydrogels

as a kind of three-dimensional (3D) network of polymer chains constructed by physical or chemical crosslinkers

possess significant potentials in wound healing

drug delivery

and tissue engineering. In recent years

stimuli-responsive hydrogels have received increasing interests on account of their fundamentally architectural features and controllably functional performances under various external stimuli

such as pH

temperature

electricity

redox

and light. Wherein

various hydrogels embedded with dynamic covalent crosslinking networks have been widely developed for high-performance functional materials since dynamic covalent bond could break and reform reversibly under suitable conditions

combining the reversibility of supramolecular non-covalent bond and the robustness of covalent bond. Herein

we demonstrate a facile and universal approach to create "living" controlled

in situ

gelling systems based on a thiol-disulﬁde exchange reaction. Thiol-disulﬁde exchange reaction is reversibly activated or terminated by deprotonating free thiols or protonating thiolates under different pH conditions with an "on/off" function

resulting in dissociation of shells and cross-linking of cores

and thus dynamically optimizing hydrogel structures: from solution to loose and compact hydrogels in macroscopic dimensions. This "living" controlled

in situ

gelation process can be optionally activated

controllably terminated and interrupted

and reinitiated by external stimuli whenever needed. Associated with an inverse emulsion technique

the controlled cross-linking strategy can be utilized to produce micro/nanoscale hydrogels in a conﬁned space with flexible architectures and designable performances. Under this circumstance

multilayered hydrogel particles with each tailor-made layer are also prepared using the controlled

in situ

gelation method in association with a seed emulsion technique. By tailoring thiol-disulﬁde exchange reaction rate in a dilute aqueous solution

a dynamic and programmable morphology and size evolution is well-performed

via

a hierarchical self-assembly strategy

providing unique advantages to fabricate intelligent drug carriers with high loading efﬁciency. Furthermore

UV-triggered thiol-disulfide exchange reaction has been developed to prepare the hydrogels with a radical-centered disulfide exchange mechanism

opening up another cross-linking strategy for precise spatiotemporal control on a photochemical gelation process by varying irradiation time. Since these hydrogels are formed through disulﬁde shufﬂing of the cores that can be easily cleaved in response to glutathione

these tailor-made hydrogels are biocompatible

biodegradable

and easily fabricated with desired shapes

sizes

and properties in controllable drug delivery systems. In this contribution

we summarize and review this disulfide-exchange-based cross-linking strategy on acquisition of smart hydrogels with adjustable structures and ﬁne-tunable properties in widely biomedical applications.

关键词

双硫键交换可控交联刺激响应性水凝胶生物医用

Keywords

Disulfide exchangeControlled cross-linkingStimuli-responsive hydrogelsBiomedical application

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