Department of Applied Physics, University of Eastern Finland, P.O. Box 1627, FI-70211 Kuopio, Finland.
Langmuir. 2012 Jul 17;28(28):10573-83. doi: 10.1021/la301642w. Epub 2012 Jul 2.
Oxidation is the most commonly used method of passivating porous silicon (PSi) surfaces against unwanted reactions with guest molecules and temporal changes during storage or use. In the present study, several oxidation methods were compared in order to find optimal methods able to generate inert surfaces free of reactive hydrides but would cause minimal changes in the pore structure of PSi. The studied methods included thermal oxidations, liquid-phase oxidations, annealings, and their combinations. The surface-oxidized samples were studied by Fourier transform infrared spectroscopy, isothermal titration microcalorimetry, nitrogen sorption, ellipsometry, X-ray diffraction, electron paramagnetic resonance spectroscopy, and scanning electron microscopy imaging. Treatment at high temperature was found to have two advantages. First, it enables the generation of surfaces free of hydrides, which is not possible at low temperatures in a liquid or a gas phase. Second, it allows the silicon framework to partially accommodate a volume expansion because of oxidation, whereas at low temperature the volume expansion significantly consumes the free pore volume. The most promising methods were further optimized to minimize the negative effects on the pore structure. Simple thermal oxidation at 700 °C was found to be an effective oxidation method although it causes a large decrease in the pore volume. A novel combination of thermal oxidation, annealing, and liquid-phase oxidation was also effective and caused a smaller decrease in the pore volume with no significant change in the pore diameter but was more complicated to perform. Both methods produced surfaces that were not found to react with a model drug cinnarizine in isothermal titration microcalorimetry experiments. The study enables a reasonable choice of oxidation method for PSi applications.
氧化是最常用的方法,用于钝化多孔硅(PSi)表面,防止与客体分子发生不需要的反应,并防止在储存或使用过程中发生时间变化。在本研究中,比较了几种氧化方法,以找到能够生成无反应性氢化物的惰性表面但对 PSi 孔结构变化最小的最佳方法。研究的方法包括热氧化、液相氧化、退火及其组合。通过傅里叶变换红外光谱、等温滴定微量热法、氮气吸附、椭圆光度法、X 射线衍射、电子顺磁共振波谱和扫描电子显微镜成像研究了表面氧化的样品。研究发现,高温处理有两个优点。首先,它能够生成无氢化物的表面,这在液相或气相中低温下是不可能的。其次,它允许硅骨架部分适应由于氧化引起的体积膨胀,而在低温下,体积膨胀会显著消耗自由孔体积。进一步优化了最有前途的方法,以最小化对孔结构的负面影响。虽然简单的 700°C 热氧化会导致孔体积大幅减少,但它被发现是一种有效的氧化方法。热氧化、退火和液相氧化的新组合也很有效,导致孔体积减少较小,孔径没有明显变化,但操作更为复杂。两种方法都产生了表面,在等温滴定微量热实验中未发现与模型药物肉桂嗪发生反应。该研究为 PSi 应用提供了合理的氧化方法选择。
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