Modification of the Stöber Process by a Polyazamacrocycle Leading to Unusual Core-Shell Silica Nanoparticles
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文摘
In the view of designing functional nanoparticles, the encapsulation of 1,4,7,10-tetraazacyclododecane (cyclen)within silica nanoparticles using the Stöber process was studied. In the presence of cyclen and tetraethoxysilane(TEOS), silica particles exhibiting an unusual core-shell structure were obtained. On then basis of TEM, DLS, andNMR data, we suggest that the particle core is constituted of hybrid primary nanoparticles resulting from cyclen-silicainteractions, whereas the shell formation results from further condensation of unreacted silica precursors. Controlexperiments performed with the zinc-cyclen complex and ammonia addition suggest that cyclen-TEOS interactionsarise from the activation of the silicon alkoxide hydrolysis with the polyazamacrocycle amine groups. These data arediscussed in the context of silica biomineralization mechanisms, where polyamine/silica interactions have been shownto play a major role. Moreover, the possibility to control the size and the structure of these nanoparticles makes thempromising materials for pharmaceutical applications.

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