Key Laboratory of Drinking Water Science and Technology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences , Beijing 100085, China.
Environ Sci Technol. 2015 Feb 3;49(3):1690-7. doi: 10.1021/es503729h. Epub 2015 Jan 23.
Fe2O3 and/or Al2O3 were supported on mesoporous SBA-15 by wet impregnation and calcinations with AlCl3 and FeCl3 as the metal precursor and were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared spectra (FTIR) of adsorbed pyridine. Fe2O3/Al2O3@SBA-15 was found to be highly effective for the mineralization of ibuprofen aqueous solution with ozone. The characterization studies showed that Al-O-Si was formed by the substitution of Al(3+) for the hydrogen of surface Si-OH groups, not only resulting in high dispersion of Al2O3 and Fe2O3 on SBA-15, but also inducing the greatest amount of surface Lewis acid sites. By studies of in situ attenuated total reflection FTIR (ATR-FTIR), in situ Raman, and electron spin resonance (ESR) spectra, the chemisorbed ozone was decomposed into surface atomic oxygen species at the Lewis acid sites of Al(3+) while it was converted into surface adsorbed (•)OHads and O2(•-) radicals at the Lewis acid sites of Fe(3+). The combination of both Lewis acid sites of iron and aluminum onto Fe2O3/Al2O3@SBA-15 enhanced the formation of (•)OHads and O2(•-) radicals, leading to highest reactivity. Mechanisms of catalytic ozonation were proposed for the tested catalysts on the basis of all the experimental information.
Fe2O3 和/或 Al2O3 通过浸渍法负载在介孔 SBA-15 上,并使用 AlCl3 和 FeCl3 作为金属前驱体进行煅烧,通过 X 射线衍射(XRD)、X 射线光电子能谱(XPS)和吸附吡啶的傅里叶变换红外光谱(FTIR)进行了表征。发现 Fe2O3/Al2O3@SBA-15 对臭氧氧化布洛芬水溶液的矿化非常有效。表征研究表明,Al-O-Si 是通过 Al(3+) 取代表面 Si-OH 基团中的氢形成的,这不仅导致 Al2O3 和 Fe2O3 在 SBA-15 上高度分散,而且还诱导了最多的表面路易斯酸位。通过原位衰减全反射傅里叶变换红外(ATR-FTIR)、原位拉曼和电子顺磁共振(ESR)谱研究,化学吸附的臭氧在 Al(3+) 的路易斯酸位上分解为表面原子氧物种,而在 Fe(3+) 的路易斯酸位上转化为表面吸附的(•)OHads 和 O2(•-) 自由基。Fe2O3/Al2O3@SBA-15 上的铁和铝的路易斯酸位的组合增强了(•)OHads 和 O2(•-) 自由基的形成,从而导致了最高的反应性。根据所有实验信息,提出了用于测试催化剂的催化臭氧化反应机理。