Enzymatic synthesis of temperature-responsive poly(N-vinylcaprolactam) microgels with glucose oxidase,Green Chemistry

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Enzymatic synthesis of temperature-responsive poly(N-vinylcaprolactam) microgels with glucose oxidase
Green Chemistry ( IF 9.3 ) Pub Date : 2017-12-06 00:00:00 , DOI: 10.1039/c7gc03111d
Elisabeth Gau _{1,

2,

3,

4,

5} , Franziska Flecken _{1,

2,

3,

4,

5} , Agnieszka Natalia Ksiazkiewicz _{1,

2,

3,

4,

5} , Andrij Pich _{1,

2,

3,

4,

5}

Affiliation

In this work we report for the first time facile enzymatic synthesis of aqueous temperature-responsive poly(N-vinylcaprolactam) (PVCL) microgels with a glucose oxidase (GOx)-based initiation system. GOx catalyzes the oxidation of β-D-glucose to D-glucono-lactone and hydrogen peroxide by the consumption of molecular oxygen. The addition of ferrous ions (Fe²⁺) induces the formation of hydroxyl radicals from the hydrogen peroxide, which act as initiating species for the microgel synthesis. PVCL microgels were synthesized by precipitation polymerization initiated by the enzyme and a conventional azo-initiator 2,2′-azobis(N-(2-carboxyethyl)-2-methylpropionamidine) tetrahydrate (ACMA) (reference). In the performed polymerization runs, the content of the crosslinker N,N′-methylenebisacrylamide (BIS) as well as the amounts of the GOx/Glu/Fe²⁺ and conventional azo-initiator ACMA were varied. The polymerization process was analyzed by reaction calorimetry and it was found that enzymatically initiated polymerization is slower compared to the conventional process, and leads to lower polymer yields. The nucleation and growth of the microgels was investigated with in situ dynamic light scattering. Dynamic light scattering experiments performed at different temperatures confirmed the temperature-responsive behavior of the obtained PVCL microgels. We demonstrate that the use of enzymes in precipitation polymerization leads to the encapsulation of enzymes in formed microgels. After the GOx-induced polymerization and purification of the microgels, high enzyme activity could be determined in the microgels, enabling facile synthesis of core–shell microgels and interesting application possibilities.

中文翻译：

用葡萄糖氧化酶酶促合成温度响应性聚（N-乙烯基己内酰胺）微凝胶

在这项工作中，我们首次报告了基于葡萄糖氧化酶（GOx）的引发系统的水性温度响应性聚（N-乙烯基己内酰胺）（PVCL）微凝胶的简便酶促合成。的GOx催化β-氧化d葡萄糖至d -glucono内酯和过氧化氢的分子氧的消耗。亚铁离子（Fe ²⁺）的添加会导致过氧化氢形成羟基自由基，而后者是微凝胶合成的引发物种。PVCL微凝胶是通过酶和常规偶氮引发剂2,2'-azobis（N-（2-羧乙基）-2-甲基丙ion）四水合物（ACMA）（参考）。在进行的聚合操作中，改变交联剂N，N′-亚甲基双丙烯酰胺（BIS）的含量以及GOx / Glu / Fe ²⁺和常规偶氮引发剂ACMA的量。通过反应量热法对聚合过程进行了分析，发现与常规方法相比，酶引发的聚合反应较慢，并且导致较低的聚合物产率。用原位研究微凝胶的成核和生长动态光散射。在不同温度下进行的动态光散射实验证实了所获得的PVCL微凝胶的温度响应行为。我们证明了在沉淀聚合中使用酶会导致所形成的微凝胶中酶的包封。在GOx诱导的微凝胶聚合和纯化后，可以确定微凝胶中的高酶活性，从而可以轻松地合成核壳微凝胶和有趣的应用可能性。

更新日期：2018-01-22

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