Smith Emily Asenath, Chen Wei
Chemistry Department, Mount Holyoke College, South Hadley, MA 01075, USA.
Langmuir. 2008 Nov 4;24(21):12405-9. doi: 10.1021/la802234x. Epub 2008 Oct 4.
Aminosilanes are common coupling agents used to functionalize silica surfaces. A major problem in applications of 3-aminopropylsilane-functionalized silica surfaces in aqueous media was encountered: the loss of covalently attached silane layers upon exposure to water at 40 degrees C. This is attributed to siloxane bond hydrolysis catalyzed by the amine functionality. To address the issue of loss of surface functionality and to find conditions where hydrolytically stable amine-functionalized surfaces can be prepared, silanization with different types of aminosilanes was carried out. Hydrolytic stability of the resulting silane-derived layers was examined as a function of reaction conditions and the structural features of the aminosilanes. Silane layers prepared in anhydrous toluene at elevated temperature are denser and exhibit greater hydrolytic stability than those prepared in the vapor phase at elevated temperature or in toluene at room temperature. Extensive loss of surface functionality was observed in all 3-aminopropylalkoxysilane-derived layers, independent of the number and the nature of the alkoxy groups. The hydrolytic stability of aminosilane monolayers derived from N-(6-aminohexyl)aminomethyltriethoxysilane (AHAMTES) indicates that the amine-catalyzed detachment can be minimized by controlling the length of the alkyl linker in aminosilanes.
氨基硅烷是用于使二氧化硅表面功能化的常见偶联剂。在3-氨丙基硅烷功能化的二氧化硅表面在水性介质中的应用中遇到了一个主要问题:在40摄氏度下接触水时,共价连接的硅烷层会损失。这归因于胺官能团催化的硅氧烷键水解。为了解决表面功能丧失的问题并找到可以制备水解稳定的胺功能化表面的条件,进行了用不同类型的氨基硅烷进行硅烷化的操作。研究了所得硅烷衍生层的水解稳定性与反应条件和氨基硅烷结构特征的关系。在无水甲苯中于高温下制备的硅烷层比在高温下以气相或在室温下于甲苯中制备的硅烷层更致密,并且表现出更高的水解稳定性。在所有3-氨丙基烷氧基硅烷衍生的层中均观察到表面功能的大量丧失,这与烷氧基的数量和性质无关。由N-(6-氨基己基)氨基甲基三乙氧基硅烷(AHAMTES)衍生的氨基硅烷单层的水解稳定性表明,通过控制氨基硅烷中烷基连接基的长度,可以使胺催化的脱离最小化。