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Self-assembled bionanoparticle polymer conjugates for building soft composite membranes

机译：自组装的生物纳米粒子聚合物共轭物，用于构建柔软的复合膜

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摘要

This project was focused on building a smart nanoporous membrane based on an assembly of bionanoconjugates. Horse spleen ferritin was chosen as a model protein scaffold to graft thermoresponsive polymers as Poly(N-isopropylacrylamide)(PNIPAAm) to it using the grafting from approach. PNIPAAm is a well known thermo-responsive polymer exhibiting a LCST of 32±C. After developing the well controlled atom transfer radical polymerization (ATRP) of NIPAAm in water at low temperature, the in-situ grafting of PNIPAAm from the ferritin was achieved. The grafting from approach consisted of two steps: the modification of ferritin into a macro-initiator by coupling the N-hydroxysuccinimide activated 2-bromo isobutyric acid ATRP initiator to the 72 addressable epsilon-amino end groups around ferritin polypeptide chains. It allows the modification of the majority of the amino sites of ferritin and induces a polymerization resulting in a higher grafting density. The condition of this chemistry has to be mild to prevent the denaturation of the proteins. The challenge was the preparation of monomeric conjugates with low polydispersity as ferritin aggregates in solution and perturbs the polymerization process. The resulting conjugates are well defined and show a thermo-responsive behavior with a Tc of about 31.5 ±C. The building of the membrane requires the crosslinking of the polymer matrix. The crosslinking was realized by a random copolymerization of NIPAAm with the monomer DMIAAm, (2-(dimethylmaleimido)-N-ethylacrylamide), a photocrosslinker. This photocrosslinker hosts a maleimide group able to form cyclobutane rings activated of UV irradiation and a sensitizer thioxanthone. The photocrosslinker is fully assimilated in the copolymer and decreases the lower critical solution temperature depending on its ratio. The assembly of the ferritin-P(NIPAAm-DMIAAm) conjugates at the solid-liquid interfaces on a mica sheet or silicon wafer creates a homogeneous thin polymer protein film. After crosslinking underUV irradiation while cooling the sample, the polymer matrix undergoes protein denaturation by the use of chaotropic agents and temperature to create nanopores in the membrane. The final membrane is a thin polymer film with monodisperse pores of about 16 nm of diameter and 2 nm depth carrying different functional groups. Such conjugates can also be assembled at the liquid-liquid interfaces forming porous micro-capsules as they reduce the interfacial tension and are able to stabilize oil droplets in solution. The ferritin-P(NIPAAm-DMIAAm) conjugates are interesting building blocks with adjustable properties able to produce functional and switchable nanoporous membranes and capsules.
机译：这个项目的重点是建立一个基于生物纳米共轭物组装的智能纳米多孔膜。选择马脾铁蛋白作为模型蛋白支架，使用接枝方法将聚（N-异丙基丙烯酰胺）（PNIPAAm）接枝到热响应性聚合物上。 PNIPAAm是一种众所周知的热响应聚合物，其LCST为32±C。在低温条件下开发了良好控制的NIPAAm原子转移自由基聚合（ATRP）之后，实现了从铁蛋白原位接枝PNIPAAm。该方法的接枝包括两个步骤：通过将N-羟基琥珀酰亚胺活化的2-溴异丁酸ATRP引发剂与铁蛋白多肽链周围的72个可寻址的ε-氨基端基偶联，将铁蛋白修饰为大分子引发剂。它可以修饰铁蛋白的大部分氨基，并引起聚合反应，从而导致更高的接枝密度。这种化学反应的条件必须温和，以防止蛋白质变性。挑战在于制备低多分散性单体共轭物，因为铁蛋白在溶液中聚集并扰乱了聚合过程。所得的缀合物定义明确，并显示出约31.5±C的Tc的热响应行为。膜的构建需要聚合物基质的交联。交联是通过NIPAAm与单体DMIAAm（2-（二甲基马来酰亚胺基）-N-乙基丙烯酰胺）（一种光交联剂）的无规共聚来实现的。该光交联剂具有能够形成被紫外线照射激活的环丁烷环的马来酰亚胺基和敏化剂噻吨酮。光交联剂在共聚物中被完全吸收，并根据其比例降低了较低的临界溶液温度。铁蛋白-P（NIPAAm-DMIAAm）共轭物在云母片或硅片上的固液界面处组装，形成均匀的聚合物蛋白薄膜。在紫外线照射下交联并冷却样品后，通过使用离液剂和温度使聚合物基质发生蛋白质变性，从而在膜上形成纳米孔。最终的膜是薄聚合物膜，具有直径约16 nm和深度2 nm的单分散孔，带有不同的官能团。这样的缀合物还可以在液-液界面处组装，形成多孔微胶囊，因为它们降低了界面张力并且能够稳定溶液中的油滴。铁蛋白-P（NIPAAm-DMIAAm）共轭物是有趣的构建基块，具有可调节的特性，能够产生功能性和可转换的纳米多孔膜和胶囊。

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    Mougin Nathalie Céline;

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  • 年度 2010
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