Journal
ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 49, Issue 3, Pages 1690-1697Publisher
AMER CHEMICAL SOC
DOI: 10.1021/es503729h
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Funding
- National Natural Science Foundation of China [21125731, 51138009, 51221892, 51278527]
- Chinese Academy of Sciences [YSW2013A02]
- Grants-in-Aid for Scientific Research [14F04734] Funding Source: KAKEN
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Fe2O3 and/or Al2O3 were supported on mesoporous SBA-15 by wet impregnation and calcinations with AlC(l)3 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 Al3+ 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 Al3+ while it was converted into surface adsorbed (OHads)-O-center dot and O-2(-) radicals at the Lewis acid sites of Fe3+. The combination of both Lewis acid sites of iron and aluminum onto Fe2O3/Al2O3@SBA-15 enhanced the formation of (OHads)-O-center dot and O-2(-) radicals, leading to highest reactivity. Mechanisms of catalytic ozonation were proposed for the tested catalysts on the basis of all the experimental information.
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