Schmidt Sonja, Alberti Sebastián, Vana Philipp, Soler-Illia Galo J A A, Azzaroni Omar
Georg-August-Universität Göttingen, Institut für Physikalische Chemie, Tammannstr. 6, 37077, Göttingen, Germany.
Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas (INIFTA), Departamento de Química, Facultad de Ciencias Exactas, Universidad Nacional de La Plata, CONICET, CC. 16 Suc. 4, La Plata, 1900, Argentina.
Chemistry. 2017 Oct 17;23(58):14500-14506. doi: 10.1002/chem.201702368. Epub 2017 Sep 12.
Rational design and elaborate modular construction of interfacial architectures in which molecular transport is mediated by responsive/adaptive nanostructures has become a growing and fertile field of research in supramolecular materials chemistry. This work presents, for the first time, the use of PNIPAM-capped mesoporous silica thin films as thermosensitive cation-selective mesochannels. Thus far, this feature has only been observed in thermosensitive biological channels. The interfacial architecture created here accomplishes its specific functions through the concerted or simultaneous action of spatially addressed subunits with temperature response and ion exclusion capabilities. The thermo-perm-selectivity effect stems from the synergistic interplay between the pH-dependent electrostatic characteristics of the silica scaffold and the thermo-controlled steric effects introduced by the capping brush layer. It is hoped that the "nanoarchitectonic" approach presented here will provide new routes toward the generation of heterosupramolecular nanosystems displaying addressable transport properties similar to those encountered in biological ion channels.
在超分子材料化学领域,通过响应性/适应性纳米结构介导分子传输的界面架构的合理设计与精细模块化构建已成为一个不断发展且成果丰硕的研究领域。这项工作首次展示了使用聚N-异丙基丙烯酰胺封端的介孔二氧化硅薄膜作为热敏阳离子选择性介孔通道。到目前为止,这一特性仅在热敏生物通道中被观察到。此处构建的界面架构通过具有温度响应和离子排斥能力的空间寻址亚基的协同或同时作用来实现其特定功能。热渗透选择性效应源于二氧化硅支架的pH依赖性静电特性与封端刷层引入的热控空间效应之间的协同相互作用。希望这里提出的“纳米结构”方法将为生成具有类似于生物离子通道中可寻址传输特性的异质超分子纳米系统提供新途径。