Formation of three-dimensional hydrogel multilayers using enzyme-mediated redox chain initiation.
Formation of three-dimensional hydrogel multilayers using enzyme-mediated redox chain initiation.
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DOI：
10.1021/am100275n
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发表时间：
2010-07
影响因子：
9.5
通讯作者：
Bowman, Christopher N.
中科院分区：
文献类型：
--
作者：
Johnson, Leah M.;DeForest, Cole A.;Pendurti, Aishwarya;Anseth, Kristi S.;Bowman, Christopher N.
关键词：
酶介导的氧化还原链起始涉及葡萄糖氧化酶（GOX）在迭代溶液浸包技术，以聚合多个，三维水凝胶层在温和的水条件下，在环境温度和氧气水平。据我们所知，顺序酶介导的浸渍涂层导致界面自由基链聚合和随后形成的三维水凝胶层之前尚未被探索过。共形的、微米尺度的、均匀的聚乙二醇（PEG）基水凝胶层在几秒钟内聚合，并在水中孵育16周后保持安全结合。在聚合反应期间，还实现了将小分子（即，罗丹明- b丙烯酸酯，丙烯酸荧光素）或荧光纳米颗粒掺入交联水凝胶层。在2-羟乙基丙烯酸酯(HEA)/PEG575双丙烯酸酯单体聚合过程中，使用gox介导的引发反应，将直径0.2 μm的纳米颗粒包封到水凝胶中，对聚合动力学的影响最小，最终丙烯酸酯转化率在几分钟内达到95%（±1%）。这种界面氧化还原方法所提供的时间控制和空间定位导致在15和120 s浸泡时间内分别聚合出150（±10）μm和650（±10）μm之间的均匀次级层。此外，将初始水凝胶底物中peg575的含量从10%增加到50%，由于水凝胶界面葡萄糖浓度降低，后续层厚度从690（±30）μm减少到490（±10）μm。通过在水凝胶底物上使用gox介导的界面聚合，在葡萄糖的存在下进行初始光聚合，可以将不同的引发机制顺序地结合在一起。严格控制层厚度，结合快速、水溶性和温和的聚合，将很容易有利于需要形成分层、复杂和三维聚合物结构的应用。
Enzyme-mediated redox chain initiation involving glucose oxidase (GOX) was employed in an iterative solution dip-coating technique to polymerize multiple, three-dimensional hydrogel layers using mild aqueous conditions at ambient temperature and oxygen levels. To our knowledge, sequential enzyme-mediated dip-coating resulting in an interfacial radical chain polymerization and subsequent formation of three-dimensional hydrogel layers has not been previously explored. Conformal, micron-scale, uniform poly(ethylene glycol) (PEG)-based hydrogel layers were polymerized within seconds and remained securely associated after incubation in water for 16 weeks. Incorporation of either small molecules (i.e., rhodamine-B acrylate, fluorescein acrylate) or fluorescent nanoparticles into crosslinked hydrogel layers during the polymerization reaction was also achieved. The encapsulation of 0.2 μm- diameter nanoparticles into hydrogels during polymerization of a 2-hydroxyethyl acrylate (HEA)/PEG575 diacrylate monomer formulation, using the GOX-mediated initiation, resulted in minimal effects on polymerization kinetics, with final acrylate conversions of 95% (±1%) achieved within minutes. The temporal control and spatial localization afforded by this interfacial redox approach resulted in the polymerization of uniform secondary layers ranging between 150 (±10) μm and 650 (±10) μm for 15 and 120 s immersion times, respectively. Moreover, increasing the PEG575-fraction within the initial hydrogel substrate from 10% to 50% decreased the subsequent layer thicknesses from 690 (±30) μm to 490 (±10) μm owing to lowered glucose concentration at the hydrogel interface. The ability to sequentially combine differing initiation mechanisms with this coating approach was achieved by using GOX-mediated interfacial polymerization on hydrogel substrates initially photopolymerized in the presence of glucose. The strict control of layer thicknesses combined with the rapid, water soluble, and mild polymerization will readily benefit applications requiring formation of stratified, complex, and three-dimensional polymer structures.
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影响因子：
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作者：
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通讯作者：
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影响因子：
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