Xiang Sanming, Zhou Yuming, Zhang Yiwei, Zhang Zewu, Sheng Xiaoli, Zhou Shijian, Yang Zunbing
School of Chemistry and Chemical Engineering, Southeast University, Nanjing 211189, P. R. China.
Dalton Trans. 2014 Jul 28;43(28):11039-47. doi: 10.1039/c4dt00882k.
A novel hollow tubular SiO2-Au catalyst with a mesoporous structure (HTMS) was successfully fabricated by a combination of the sol-gel and calcination processes. This method involves the preparation of modified MWCNTs, the sequential deposition of Au and then silica layers through the sol-gel processes, and finally the calcination at the desired temperature to remove the MWCNTs. The obtained samples were characterized by several techniques, such as N2 adsorption-desorption isotherms, transmission electron microscopy, energy-dispersive X-ray spectroscopy analysis, UV-Vis spectra, X-ray diffraction and Thermogravimetric Analysis (TGA). The results established that a different calcination temperature has an obvious influence on the morphology and structure of the final hollow tubular. When the temperature is 550 °C, the obtained materials exhibit the distinctly tubular structure because of the decomposition of MWCNTs and the preservation of hollow tubes. Furthermore, in the catalyst system, the mesoporous silica layer can act as the physical barrier to resist the agglomeration and sintering of Au nanoparticles even after being subjected to harsh treatments up to 650 °C. In our experiments, the catalytic activities of HTMS SiO2-Au were investigated by photometrically monitoring the reduction of p-nitrophenol (p-NPh) by an excess of NaBH4. It was found that the prepared HTMS SiO2-Au catalysts exhibited a high catalytic activity and this sample could be easily recycled without a decrease of the catalytic activities in the reaction.
通过溶胶 - 凝胶法和煅烧工艺相结合,成功制备了一种具有介孔结构的新型中空管状SiO₂ - Au催化剂(HTMS)。该方法包括制备改性多壁碳纳米管,通过溶胶 - 凝胶工艺依次沉积金层和二氧化硅层,最后在所需温度下煅烧以去除多壁碳纳米管。通过多种技术对所得样品进行了表征,如N₂吸附 - 脱附等温线、透射电子显微镜、能量色散X射线光谱分析、紫外 - 可见光谱、X射线衍射和热重分析(TGA)。结果表明,不同的煅烧温度对最终中空管的形态和结构有明显影响。当温度为550℃时,由于多壁碳纳米管的分解和中空管的保留,所得材料呈现出明显的管状结构。此外,在催化剂体系中,即使在高达650℃的苛刻处理后,介孔二氧化硅层也可以作为物理屏障来抵抗金纳米颗粒的团聚和烧结。在我们的实验中,通过光度监测过量NaBH₄对对硝基苯酚(p - NPh)的还原反应来研究HTMS SiO₂ - Au的催化活性。结果发现,制备的HTMS SiO₂ - Au催化剂表现出高催化活性,并且该样品在反应中可以很容易地循环使用而不降低催化活性。