Darga Alexander, Kecht Johann, Bein Thomas
Department of Chemistry and Biochemistry, University of Munich, Butenandtstrasse 5-13 (E), 81377 Munich, Germany.
Langmuir. 2007 Dec 18;23(26):12915-22. doi: 10.1021/la701962b. Epub 2007 Nov 15.
The incorporation of organic moieties into siliceous frameworks leads to a wide variety of adsorbate-adsorbent interactions including weak van-der-Waal attractions as well as strong interactions such as Coulomb forces. Depending on the desired properties of such substituted highly porous matrix materials, optimized synthesis routes can be established to enhance the desired internal pore surface-affinity toward certain volatile compounds. On the basis of a fundamental knowledge of the host-guest system, sorption-related applications may benefit from individually fine-tuned and modified sample materials. The sorption isotherms of vaporized toluene on nonmodified and phenyl-functionalized mesoporous silica samples were determined on an acoustic wave device at different temperatures. The mesoporous silica was modified by in situ co-condensation and postsynthesis grafting approaches, respectively. All samples were thoroughly characterized by nitrogen sorption, thermogravimetric analysis (TGA), scanning and transmission electron microscopy (SEM, TEM), solid-state nuclear magnetic resonance (29Si NMR), dynamic light scattering (DLS), Raman spectroscopy, and toluene adsorption on a quartz crystal microbalance (QCM). The different heats of adsorption of toluene on the various modified silica surfaces obtained by the sorption data make it possible to gain additional information about the degree and type of surface functionalization. It is thus demonstrated that QCM studies can be a powerful and convenient tool for efficient investigations of functionalized mesoporous silica particles that yield valuable quantitative information on molecule-surface interactions.
将有机部分引入硅质骨架会导致多种吸附质 - 吸附剂相互作用,包括弱范德华引力以及诸如库仑力等强相互作用。根据此类取代的高孔隙率基质材料所需的性质,可以建立优化的合成路线,以增强对某些挥发性化合物所需的内部孔表面亲和力。基于主客体系统的基础知识,与吸附相关的应用可能会受益于单独微调及改性的样品材料。在不同温度下,使用声波装置测定了汽化甲苯在未改性和苯基官能化的介孔二氧化硅样品上的吸附等温线。介孔二氧化硅分别通过原位共缩合和后合成接枝方法进行改性。所有样品均通过氮气吸附、热重分析(TGA)、扫描和透射电子显微镜(SEM、TEM)、固态核磁共振(29Si NMR)、动态光散射(DLS)、拉曼光谱以及在石英晶体微天平(QCM)上进行甲苯吸附进行了全面表征。通过吸附数据获得的甲苯在各种改性二氧化硅表面上不同的吸附热,使得获取有关表面功能化程度和类型的额外信息成为可能。因此证明,QCM研究可以成为一种强大且便捷的工具,用于高效研究功能化介孔二氧化硅颗粒,这些颗粒能提供有关分子 - 表面相互作用的有价值的定量信息。