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Prevention of the Aggregation of Nanoparticles during the Synthesis of Nanogold-Containing Silica Aerogels

机译:含纳米金的二氧化硅气凝胶的合成过程中防止纳米粒子的聚集

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摘要

Nanogold is widely used in many areas of physics and chemistry due to its environment-sensitive plasmon resonance absorption. The immobilization of gold nanoparticles in highly porous silica aerogel offers an attractive alternative to liquid gold solutions as they show a mechanically stable structure, are permeable to gases, and can even be used at elevated temperatures. We have found that the commercially available citrate-stabilized 10 nm gold nanoparticles may suffer from aggregation prior to or under the base-catalyzed gelation process of tetramethoxy silane. In the wet gels, Au particles increased in size, changed shape, and demonstrated the loss of plasmon resonance absorption, due to the formation of larger aggregates. We have studied a range of water-miscible organic solvents, stabilizing agents, and the gelation conditions to minimize changes from occurring in the aerogel setting and the supercritical drying process. It has been found that atmospheric carbon dioxide has a significant effect on aggregation, and it cannot be entirely excluded under normal synthetic conditions. Methanol resulted in an increase in the particle size only, while dimethyl sulfoxide, dimethylformamide, and urea changed the shape of nanoparticles to rod-like shapes, and diols led to an increase in both size and shape. However, using the polymeric stabilizer poly(vinyl pyrrolidone) efficiently prevented the aggregation of the particles, even in the presence of high concentrations of carbon dioxide, and allowed the production of nanoAu containing silica aerogels in a single step, without the modification of technology.
机译:纳米金由于其对环境敏感的等离振子共振吸收而被广泛用于物理和化学的许多领域。将金纳米颗粒固定在高度多孔的二氧化硅气凝胶中,是液态金溶液的一种有吸引力的替代方法,因为它们显示出机械稳定的结构,可渗透气体,甚至可以在高温下使用。我们已经发现,市售的柠檬酸盐稳定的10nm金纳米颗粒在四甲氧基硅烷的碱催化的胶凝过程之前或之下可能遭受聚集。在湿凝胶中,由于形成了较大的聚集体,Au颗粒尺寸增大,形状改变,并显示出等离子体共振吸收的损失。我们研究了多种与水混溶的有机溶剂,稳定剂和胶凝条件,以最大程度地减少气凝胶凝结和超临界干燥过程中发生的变化。已经发现,大气中的二氧化碳对聚集具有显着的影响,并且在正常的合成条件下不能将其完全排除。甲醇仅导致粒径增加,而二甲基亚砜,二甲基甲酰胺和尿素将纳米颗粒的形状改变为棒状,而二醇导致尺寸和形状均增加。然而,即使在存在高浓度二氧化碳的情况下,使用聚合物稳定剂聚(乙烯基吡咯烷酮)也有效地防止了颗粒的聚集,并且允许在不改变技术的情况下一步生产含纳米金的二氧化硅气凝胶。

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