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Fundamental research on design of nano-device using self-oscillating gel

自振荡凝胶纳米器件设计基础研究

基本信息

批准号：
15205027
负责人：
YOSHIDA Ryo
金额：
$ 32.78万
依托单位：
The University of Tokyo
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (A)
财政年份：
2003
资助国家：
日本
起止时间：
2003 至 2006
项目状态：
已结题

项目摘要

As a novel biomimetic polymer, we have been studying the polymer with an automonous self-oscillating function by utilizing oscillating chemical reactions. We succeeded in developing a novel self-oscillating polymer and gels by utilizing the Belousov-Zhabotinsky (BZ) reaction. The self-oscillating polymer is composed of poly(N-isopropylacrylamide) (PNIPAAm), in which Ru(bpy)_3 is incorporated as a catalyst for the BZ reaction. Under the coexistence of the reactants (malonic acid, sodium bromate, and nitric acid), the polymer undergoes spontaneous cyclic soluble-insoluble changes or swelling-deswelling changes (in the case of gel) without any on-off switching of external stimuli. To cause the self-oscillation of the polymer under physiological condition without utilizing non-biorelated BZ substrates, we have been attempting to construct the build-in system where the substrates other than organic acid are incorporated into the polymer itself. As the first step, acrylamide-2-methylpropanes … More ulfonic acid (AMPS) was incorporated into the poly(NIPAAm-co-Ru(bpy)_3) as the pH-control site. As the next step, we have attempted to introduce the oxidizing agent into the polymer. Methacrylamidopropyltrimethylammonium chloride (MAPTAC) with a positively charged group was incorporated into the poly(NIPAAm-co-Ru(bpy)_3) as a capture site for an anionic oxidizing agent (bromate ion). The bromate ion was introduced into the MAPTAC-containing polymer through ion-exchange process. By using the copolymer, self-oscillation only in the presence of organic acid was achieved. To synthesize an artificial biomachine with self-beating function which acts under physiological condition, we have developed another self-oscillating gel that can be driven by chemical energy of ATP decomposition. Anionic polymer gel with phosphoric groups, in which creatine kinase was immobilized, was prepared. When the gel was immersed in the ATP solution, the enzymatic reaction occurs in the gel and the concentration of calcium ion changes periodically. As a result, the gel repeats swelling and deswelling autonomously. Less

作为一种新型的仿生聚合物，我们利用振荡化学反应来研究具有自振荡功能的聚合物。我们利用Belousov-Zhabotinsky （BZ）反应成功地开发了一种新型自振荡聚合物和凝胶。该自振荡聚合物由聚n -异丙基丙烯酰胺（PNIPAAm）组成，其中Ru(bpy)_3作为BZ反应的催化剂。在反应物（丙二酸、溴酸钠和硝酸）共存的情况下，聚合物经历自发的可溶-不溶性变化或肿胀-肿胀变化（在凝胶的情况下），没有任何外部刺激的开关。为了在不使用非生物相关BZ底物的情况下引起聚合物在生理条件下的自振荡，我们一直在尝试构建内置系统，其中除有机酸外的底物被纳入聚合物本身。首先，在聚（NIPAAm-co-Ru(bpy)_3）中加入更多的磺酸（AMPS）作为ph控制位点。下一步，我们尝试在聚合物中加入氧化剂。带正电基团的甲基丙烯酰胺丙基三甲基氯化铵（MAPTAC）被引入聚NIPAAm-co-Ru(bpy)_3中，作为阴离子氧化剂（溴酸盐离子）的捕获位点。通过离子交换将溴酸盐离子引入到含maptac聚合物中。通过使用该共聚物，仅在有机酸存在下才实现自振荡。为了合成一种在生理条件下具有自跳动功能的人工生物机器，我们研制了一种由ATP分解化学能驱动的自振荡凝胶。制备了以肌酸激酶为固定载体的磷酸基阴离子聚合物凝胶。当凝胶浸泡在ATP溶液中时，凝胶中发生酶促反应，钙离子浓度周期性变化。因此，凝胶会自动重复肿胀和肿胀。少