Monitoring temporal evolution of silicate species during hydrolysis and condensation of silicates using mass spectrometry

被引:122
作者
Pelster, SA [1 ]
Schrader, W [1 ]
Schüth, F [1 ]
机构
[1] Max Planck Inst Kohlenforsch, D-45470 Mulheim, Germany
关键词
D O I
10.1021/ja057423r
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The first stages of solid-state formation from solution can be crucial in determining the properties of the resulting solids. We are trying to approach prenucleation reactions of silicates from an aqueous solution containing tetraalkylammoniumhydroxides (TAAOH) and tetraalkoxysilanes (TAOS) by analyzing hydrolysis and condensation using electrospray mass spectrometry (ESI MS). Time-resolved measurements were performed using different reactor systems to show the stepwise hydrolysis of the silanes and subsequent condensation of silicate monomers via oligomers to form larger units. We approached the precipitation point by varying the pH and the concentrations of the reactants. The results show the evolution of different silicate species occurring during condensation. No defined molecular entities were identified at pH values close to precipitation, which suggests that under the conditions used, solids are probably not formed from defined building blocks.
引用
收藏
页码:4310 / 4317
页数:8
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