基于适度两亲性嵌段共聚物的可注射性热致水凝胶

崔书铨; 俞麟; 丁建东

doi:10.11777/j.issn1000-3304.2018.18084

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基于适度两亲性嵌段共聚物的可注射性热致水凝胶

专论 | 更新时间：2021-01-26

- 基于适度两亲性嵌段共聚物的可注射性热致水凝胶
- Injectable Thermogels Based on Block Copolymers of Appropriate Amphiphilicity
- 高分子学报 2018年0卷第8期页码：997-1015
- 作者机构：
  
  聚合物分子工程国家重点实验室复旦大学高分子科学系　上海 200438
- 作者简介：
  
  [ "丁建东，男，1965年出生. 现为复旦大学高分子科学系教授、博士生导师，聚合物分子工程国家重点实验室主任. 1988年本科毕业于复旦大学生命科学院生物物理专业；1991年6月和1995年1月分别于复旦大学材料科学系和高分子科学系获得高分子化学与物理专业硕士和博士学位；1998年8月至1999年8月于英国剑桥大学材料系从事博士后研究. 1991年毕业留校. 教育部长江特聘教授、国家杰出青年基金获得者，入选国家“万人计划”系列的“百千万工程领军人才”，当选国际生物材料联合会会士. 主要研究领域为生物医用高分子. 科研成果“可注射性热致水凝胶”获得教育部自然科学一等奖(完成人：丁建东、俞麟)" ]
- 基金信息：
  
  国家自然科学基金(基金号 21774024，51533002)和国家重点研发计划项目(项目号 2016YFC1100300)资助()
- DOI：10.11777/j.issn1000-3304.2018.18084
  中图分类号：
- 纸质出版日期：2018-8，
  
  收稿日期：2018-3-29，
  
  修回日期：2018-5-27，
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崔书铨, 俞麟, 丁建东. 基于适度两亲性嵌段共聚物的可注射性热致水凝胶[J]. 高分子学报, 2018,0(8):997-1015.

Shu-quan Cui, Lin Yu, Jian-dong Ding. Injectable Thermogels Based on Block Copolymers of Appropriate Amphiphilicity[J]. Acta Polymerica Sinica, 2018,0(8):997-1015.
崔书铨, 俞麟, 丁建东. 基于适度两亲性嵌段共聚物的可注射性热致水凝胶[J]. 高分子学报, 2018,0(8):997-1015. DOI： 10.11777/j.issn1000-3304.2018.18084.

Shu-quan Cui, Lin Yu, Jian-dong Ding. Injectable Thermogels Based on Block Copolymers of Appropriate Amphiphilicity[J]. Acta Polymerica Sinica, 2018,0(8):997-1015. DOI： 10.11777/j.issn1000-3304.2018.18084.

摘要

部分两亲性嵌段共聚物的水溶液随温度升高呈现可逆的溶胶-凝胶转变. 如果转变温度介于室温和体温之间，该类体系可以在室温或更低温与药物或细胞混合，并可以注射；一旦注射进入体内，在体温下原位凝胶化，可以自动包裹药物或细胞，且该过程不依赖于化学反应. 由聚乙二醇和疏水的可降解聚酯构成的嵌段共聚物的水体系在合适分子量等条件下具备以上的可逆热致凝胶化特性，成为一类极有前景的新型生物医用材料，但其中仍有大量的高分子科学问题需要解决. 作者课题组十余年来在可注射热致水凝胶领域开展了系统研究：发现了聚酯-聚醚嵌段共聚物的端基效应、分子量分布效应等重要现象，总结了热致水凝胶分子设计的规律；揭示了物理凝胶化的机理，并显著扩展了可热致凝胶化聚合物的成分范围；发展了热致水凝胶面向医学应用的新策略. 本专论主要以近年来复旦大学生物医用材料课题组对聚乙二醇/聚酯类可注射性热致水凝胶体系的研究为重点，介绍该类高分子材料的物理凝胶化机理和调控规律，并根据相关动物实验结果展示其潜在的临床应用前景.

Abstract

Some amphiphilic copolymers in water can undergo a reversible sol-gel transition upon heating. If the transition temperature lies between room temperature and body temperature

the aqueous system can be readily mixed with drugs or cells at room temperature

and the mixture is injectable; the injected formulation is physically gelled at body temperature

and the gelation is free of any chemical crosslinking. This affords an amazing biomaterial type

yet many questions are open in light of fundamental research and potential clinical applications. In particular

block copolymers composed of hydrophilic poly(ethylene glycol) (PEG) and some hydrophobic biodegradable polyesters such as poly(lactide-

-glycolide) (PLGA) are of great clinical potential

yet of very unclear physical crosslinking points. This feature article summarizes the corresponding extensive investigations in the authors’ group led by Ding at Fudan University for a decade. The Ding group has found the significant effects of the end groups of the copolymer

molar mass dispersity

and other molecular parameters on thermogellability

and revealed the corresponding rules of molecular design

based on their polymer chemistry studies. For instance

with increase in

under either given number average or weight average molecule weight

the sol-gel transition temperature for some block copolymer aqueous systems could shift unidirectionally

which indicates that the effect of molecular weight distribution could not be interpreted simply from addition of the effects of molecular weight or

affords an independent adjustable parameter. The Ding group has shed light on the mechanism of their thermogelling by putting forward the model of percolated micelle network to describe the internal structure of the physical hydrogel

and extended the range of the thermogellable molecular composition of the copolymers to a large extent by establishing a blend strategy

based on their polymer physics studies. The Ding group have also put forward many strategies for the clinical applications of the thermogels using animal models

including prevention of postoperative tissue adhesion

submucosal cushion for endoscopic submucosal dissection

sustained release carriers of antitumor drugs such as camptothecin derivatives

long-acting formulations of polypeptide drugs such as exenatide in treatment of type II diabetes

and tissue engineering of cartilage. The Ding group has also laid a material basis towards potential products of medical devices and drug carriers including the appropriate way of sterilization and improvement of the handling property of the synthesized polymers. The Ding group suggest some perspectives in the end of this feather article.

关键词

两亲性嵌段共聚物物理水凝胶生物医用材料

Keywords

Amphiphilic block copolymerPhysical hydrogelBiomedical materials

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Zhu W, Ding J D . J Appl Polym Sci , . 2006 . 99 ( 5 ): 2375 - 2383.

He Yao(何垚), Pan Zhen(潘震), Ding Jiandong(丁建东). Acta Polymerica Sinica(高分子学报), 2013, (6): 755-764

Qi Y L, Qi H P, He Y, Lin W J, Li P Z, Qin L, Hu Y W, Chen L P, Liu Q S, Sun H T, Liu Q, Zhang G, Cui S Q, Hu J, Yu L, Zhang D Y, Ding J D . ACS Appl Mater Interfaces , . 2018 . 10 ( 1 ): 182 - 192.

Ding J D . Sci China Mater , . 2018 . 61 ( 8 ): 1132 - 1134 . DOI:10.1007/s40843-018-9228-4http://doi.org/10.1007/s40843-018-9228-4 .

Zhu Wen(朱文), Zhang Ying(张颍), Wang Biaobing(王标兵), Ding Jiandong(丁建东). Chemical Journal of Chinese Universities(高等学校化学学报), 2005, 2(3): 373-375

Zhu W, Wang B B, Zhang Y, Ding J D . Eur Polym J , . 2005 . 41 ( 9 ): 2161 - 2170.

Yang Z G, Ding J D . Macromol Rapid Commun , . 2008 . 29 ( 9 ): 751 - 756.

Yu L, Zhang Z, Ding J D . Macromol Res , . 2012 . 20 ( 3 ): 234 - 243.

Peng Y M, Liu Q J, He T L, Ye K, Yao X, Ding J D. Biomaterials, 2018, Doi: 10.1016/j.biomaterials.2018.04.021

Yu L, Zhang Z, Zhang H, Ding J D . Biomacromolecules , . 2010 . 11 ( 8 ): 2169 - 2178.

Lei K W, Ma Q, Yu L, Ding J D . J Mater Chem B , . 2016 . 4 ( 48 ): 7793 - 7812.

Qi Yongli(齐永丽), Lei Kewen(雷科文), Yu Lin(俞麟), Ding Jiandong(丁建东). Polymer Bulletin(高分子通报), 2016, (5): 43-51

Zhou Y Y, Zhuang Y P, Li X, Agren H, Yu L, Ding J D, Zhu L L . Chem-Eur J , . 2017 . 23 ( 32 ): 7642 - 7647.

Lei K W, Shen W J, Cao L P, Yu L, Ding J D . Chem Commun , . 2015 . 51 ( 28 ): 6080 - 6083.

Ma Q, Lei K W, Ding J, Yu L, Ding J D . Polym Chem , . 2017 . 8 ( 43 ): 6665 - 6674.

Lei K W, Chen Y P, Wang J Y, Peng X C, Yu L, Ding J D . Acta Biomater , . 2017 . 55 396 - 409.

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