Glucose-responsive Dynamic Covalent Hydrogels Based on PVA-<italic style="font-style: italic">b</italic>-PEO-<italic style="font-style: italic">b</italic>-PVA and Phenylboronic Acid Substituted PEO Crosslinker

Ting Yang; Fu-sheng Du; Zi-chen Li

doi:10.11777/j.issn1000-3304.2019.19017

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Glucose-responsive Dynamic Covalent Hydrogels Based on PVA-b-PEO-b-PVA and Phenylboronic Acid Substituted PEO Crosslinker

Research Article | 更新时间：2021-01-26

- Glucose-responsive Dynamic Covalent Hydrogels Based on PVA-b-PEO-b-PVA and Phenylboronic Acid Substituted PEO Crosslinker
  增强出版
- Acta Polymerica Sinica Vol. 50, Issue 5, Pages: 516-526(2019)
- 作者机构：
  
  北京分子科学国家研究中心高分子化学与物理教育部重点实验室北京大学化学与分子工程学院　北京 100871
- 作者简介：
- 基金信息：
- DOI：10.11777/j.issn1000-3304.2019.19017
  CLC：
- Published：2019-5，
  
  Published Online：11 April 2019，
  
  Received：25 January 2019，
  
  Revised：14 March 2019，
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Ting Yang, Fu-sheng Du, Zi-chen Li. Glucose-responsive Dynamic Covalent Hydrogels Based on PVA-b-PEO-b-PVA and Phenylboronic Acid Substituted PEO Crosslinker. [J]. Acta Polymerica Sinica 50(5):516-526(2019)
DOI：

Ting Yang, Fu-sheng Du, Zi-chen Li. Glucose-responsive Dynamic Covalent Hydrogels Based on PVA-b-PEO-b-PVA and Phenylboronic Acid Substituted PEO Crosslinker. [J]. Acta Polymerica Sinica 50(5):516-526(2019) DOI： 10.11777/j.issn1000-3304.2019.19017.

摘要

设计合成了一类含苯硼酸和氨基结构的聚环氧乙烷(PEO)大分子交联剂，利用其与含聚乙烯醇(PVA)的三嵌段共聚物PVA-

-PEO-

-PVA之间的动态共价作用，构筑得到一类在生理pH下稳定，且对葡萄糖有响应的动态共价凝胶；详细研究了交联剂用量、PVA链段长度对凝胶化过程及凝胶稳定性的影响，证明PVA链段越长、交联剂用量越高，凝胶的稳定性越高，同时这类凝胶的屈服力较高，性质上更接近固体. 凝胶在pH = 7.4，37 °C保持其结构稳定性. 进一步发现这类动态共价凝胶具有较强的结构修复能力以及对糖的响应能力，凝胶可包载蛋白质FITC-BSA，加入葡萄糖后，其释放显著加快.

Abstract

Boronic acid can form dynamic covalent boronic ester bonds with 1

2-diol or 1

3-diol moieties. This property has been used to prepare malleable and self-healing covalent polymer networks as well as glucose-responsive hydrogels. It remains a challenge to fabricate strong hydrogels with fast glucose-responsivity. Glucose-responsive dynamic covalent hydrogels were prepared by crosslinking poly(vinyl alcohol) (PVA) containing triblock copolymer and poly(ethylene oxide) (PEO) containing phenylboric acid. Specifically

we synthesized a new type of

-phenylboronic acid substituted PEO crosslinker. The feature of the crosslinker is that amino-groups are introduced to the neighboring position of boronic acid

which will accelerate the boronic ester exchange. The gelation of this crosslinker with three PVA-

-PEO-

-PVA triblock copolymers at physiological pH was examined. Time-dependent dynamic storage and loss modulus of the hydrogels were monitored by rheological measurements. Formation of hydrogels turned out be very fast after mixing the crosslinker and triblock copolymer solutions. Stable dynamic covalent hydrogels were obtained after incubating the hydrogels for 12 h. The copolymer composition

PVA chain length

and content of crosslinker were found to greatly affect the hydrogel properties. Higher polymer concentration

longer PVA chains

and more PEO crosslinker endowed hydrogels with higher modulus. Gels with high yield stress were obtained by utilizing block copolymer with longer PVA segments or adding more crosslinker. Both pH and temperature affected the hydrogel properties. The formed hydrogels displayed higher modulus at pH = 7.4 than those at pH = 6.0

and the stability of the hydrogel could still be maintained at 37 °C. In addition

the hydrogels exhibited good structural recovery ability due to the covalent dynamic crosslinking. Finally

the hydrogels could load FITC-BSA

and the release profile of FITC-BSA was accelerated in the presence of glucose.

关键词

苯硼酸聚环氧乙烷聚乙烯醇水凝胶葡萄糖响应

Keywords

Phenylboronic acidPoly(ethylene oxide)Poly(vinyl alcohol)HydrogelGlucose-responsive

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Beijing National Laboratory for Molecular Sciences,Key Laboratory of Polymer Chemistry and Physics of Ministry of Education,College of Chemistry and Molecular Engineering,Peking University

Department of Material Science and engineering, Jinan University

School of Chemistry, Xi'an Jiaotong University

University of Science and Technology of China

CAS Key Laboratory of Renewable Energy, Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development, Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences

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Glucose-responsive Dynamic Covalent Hydrogels Based on PVA-b-PEO-b-PVA and Phenylboronic Acid Substituted PEO Crosslinker

DOI：10.11777/j.issn1000-3304.2019.19017

摘要

Abstract

关键词

Keywords

references