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首页> 外文期刊>Chemistry of Materials: A Publication of the American Chemistry Society >Design of Self-Oscillating Polymer Brushes and Control of the Dynamic Behaviors
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Design of Self-Oscillating Polymer Brushes and Control of the Dynamic Behaviors

机译:自激式聚合物电刷的设计和动态行为的控制

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摘要

A polymer brush surface with autonomous function has been designed by using a self-oscillating polymer that we developed. The self-oscillation is induced by chemomechanical energy conversion from an oscillating chemical reaction (the Belousov-Zhabotinsky (BZ) reaction) to conformational changes of polymer chains. In this study, the surface nanostructure of polymer brushes were regulated and the spatiotemporal behaviors of self-oscillation were investigated. The target polymer brush surfaces were prepared through surface-initiated atom transfer radical polymerization (SI-ATRP) of N-isopropylacrylamide (NIPAAm) and N-(3-aminopropyl) methacrylamide (NAPMAm), and the subsequent conjugation of Ru(bpy)(3) to the amino group of NAPMAm. The characterization of the prepared polymer brush and the free polymer was determined by X-ray photoelectron spectroscopy, atomic force microscopy, attenuated total reflection Fourier transform infrared spectroscopy, UV-vis spectrophotometry, gel permeation chromatography, and H-1 NMR. Their dynamic properties were estimated by quartz crystal microbalance with dissipation and fluorescence microscopy. The amounts of Ru(bpy)(3) immobilized to polymer brush surfaces could be controlled by adjusting the reaction conditions of SI-ATRP and conjugating Ru(bpy)(3). Importantly, an appropriate structure of polymer brush to give stable oscillation has been indicated from image analysis of chemical wave propagation. Further, several physicochemical parameters to control the oscillating behaviors, including the rate constant of the autocatalytic reaction, the diffusion constant of the activator, and the activation energies for the reaction and diffusion, have been obtained from theoretical consideration. These results will be helpful for developing subsequent applications such as autonomous transport systems.
机译:通过使用我们开发的自振荡聚合物,设计了具有自主功能的聚合物刷表面。自振荡是由化学机械能转换引起的,该化学机械能从振荡化学反应(Beloousov-Zhabotinsky(BZ)反应)转变为聚合物链的构象变化。在这项研究中,聚合物刷的表面纳米结构受到调控,并研究了自振荡的时空行为。通过N-异丙基丙烯酰胺(NIPAAm)和N-(3-氨基丙基)甲基丙烯酰胺(NAPMAm)的表面引发的原子转移自由基聚合(SI-ATRP)以及随后的Ru(bpy)( 3)到NAPMAm的氨基。通过X射线光电子能谱,原子力显微镜,衰减全反射傅立叶变换红外光谱,紫外可见分光光度法,凝胶渗透色谱法和H-1 NMR来确定所制备的聚合物刷和游离聚合物的特征。通过具有耗散和荧光显微镜的石英晶体微量天平估算了它们的动态性能。固定在聚合物刷表面的Ru(bpy)(3)的量可以通过调整SI-ATRP的反应条件并结合Ru(bpy)(3)来控制。重要的是,已经通过化学波传播的图像分析表明了聚合物刷的适当结构以提供稳定的振动。此外,从理论上已经获得了一些控制振荡行为的物理化学参数,包括自催化反应的速率常数,活化剂的扩散常数以及反应和扩散的活化能。这些结果将有助于开发后续应用,例如自动运输系统。

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