School of Environmental Engineering, University of Seoul, Seoul 02504, Republic of Korea.
Department of Chemistry, Sungkyunkwan University, Suwon 16419, Republic of Korea.
Environ Res. 2019 May;172:649-657. doi: 10.1016/j.envres.2019.03.016. Epub 2019 Mar 7.
The catalytic oxidation of toluene with ozone at room temperature was carried out over hierarchically ordered mesoporous catalysts (CeO (meso), MnO (meso), ZrO (meso), and γ-AlO (meso)) and AlO with various textural properties and phases (γ-AlO (meso), γ-AlO (13 nm), and α-AlO) to examine the effects of the nature of the catalyst on the catalytic activity. The catalysts were characterized by N-physisorption measurements, powder X-ray diffraction, temperature programmed reduction, X-ray photoelectron spectroscopy and scanning transmission electron microscopy with energy dispersive spectroscopy. Among the ordered mesoporous catalysts, γ-AlO (meso) had the highest toluene removal efficiency because of its highest surface area and pore volume, which in turn was selected for further investigation. Manganese (Mn) was introduced to various AlO to improve the toluene removal efficiency. Comparing the Mn-loaded catalysts supported on various AlO with different crystalline phases or pore structures, Mn/γ-AlO (meso), had the highest catalytic activity as well as the highest CO/CO ratio. The higher activity was attributed to the larger surface area, weaker interaction between Mn and AlO, and larger portion of MnO phase. The increase in ozone concentration led to an improvement in the carbon balance but this enhancement was insufficient due to the deposition of by-products on the catalyst. After long term tests at room temperature, the reaction intermediates and carbonaceous deposits of the used catalysts were identified.
在室温下,采用具有不同织构性质和相态的介孔有序催化剂(CeO(meso)、MnO(meso)、ZrO(meso)和γ-AlO(meso))和 AlO(γ-AlO(meso)、γ-AlO(13nm)和α-AlO)对甲苯进行臭氧催化氧化,以考察催化剂性质对催化活性的影响。通过 N 物理吸附测量、粉末 X 射线衍射、程序升温还原、X 射线光电子能谱和扫描透射电子显微镜与能量色散光谱对催化剂进行了表征。在有序介孔催化剂中,γ-AlO(meso)具有最高的甲苯去除效率,因为其具有最高的比表面积和孔体积,因此选择其进行进一步研究。在各种 AlO 上引入锰(Mn)以提高甲苯去除效率。比较不同晶相或孔结构的负载 Mn 的催化剂,Mn/γ-AlO(meso)具有最高的催化活性和最高的 CO/CO 比。更高的活性归因于更大的比表面积、Mn 和 AlO 之间较弱的相互作用以及更大比例的 MnO 相。臭氧浓度的增加导致碳平衡的改善,但由于产物在催化剂上的沉积,这种增强是不充分的。在室温下进行长期测试后,鉴定了使用后的催化剂的反应中间体和含碳沉积物。