ABSTRACT

Iron and titanium doped γ-Al₂O₃ (γ-Fe-Ti-Al₂O₃) mesoporous catalysts were synthesized by evaporation-induced self-assembly using glucose as template, and applied to ozonation of ibuprofen in bromide-containing water. X-ray diffraction (XRD), nitrogen adsorption–desorption (BET), X-ray photoelectron spectroscopy (XPS) results showed that iron and titanium successfully doped into the skeleton of γ-Al₂O₃, uniform distribution, maintain the ordered mesoporous structure of γ-Al₂O₃, with larger specific surface area. The valence of titanium coexists with Ti⁴⁺ and Ti³⁺, and the valence of iron was Fe³⁺. Infrared spectra of chemisorbed pyridine (Py-FTIR) results showed that the doped titanium and iron into the framework position of γ-Al₂O₃ altered the surface acidity of the alumina surface, especially increasing the medium Lewis acid sites, which was conducive to the effective decomposition of ozone into active oxygen species. The γ-Fe-Ti-Al₂O₃ catalyst (Al/Fe = 25, Al/Ti = 75) enhanced the removal rate of ibuprofen in ozonation of bromide-containing water, and effectively blocked the formation of bromate. After the reaction of 60 min, the removal rate of TOC was increased from 54% of γ-Al₂O₃/O₃ to 86% with γ-Fe-Ti-Al₂O₃/O₃, while the ozonation alone was only 13%. Electron Paramagnetic Resonance (EPR) spectra showed that hydroxyl and superoxide radicals were reactive oxygen species, which was beneficial to the mineralization of organic matter. The capture experiment of Fe²⁺ ion confirmed that the electronic cycle of Fe²⁺ ion and Fe³⁺ ion was beneficial to block the formation of bromated. The addition of ibuprofen and humic acid can enhance the reduction of Fe³⁺ in the catalytic ozonation of γ-Fe-Ti-Al₂O₃, which further strengthened the blocking of bromate formation.

 抽象的

以葡萄糖为模板，通过蒸发诱导自组装合成了铁钛掺杂的γ-Al ₂ O ₃ (γ-Fe-Ti-Al ₂ O ₃ )介孔催化剂，并将其应用于布洛芬在含溴化物水中的臭氧化反应。 X射线衍射(XRD)、氮气吸附-脱附(BET)、X射线光电子能谱(XPS)结果表明铁和钛成功掺杂到γ-Al ₂ O ₃骨架中，分布均匀，保持了有序的介孔结构。 γ-Al ₂ O ₃结构，具有较大的比表面积。钛的价态为Ti ⁴⁺和Ti ³⁺共存，铁的价态为Fe ³⁺ 。化学吸附吡啶红外光谱（Py-FTIR）结果表明，γ-Al ₂ O ₃骨架位置掺杂钛和铁改变了氧化铝表面的表面酸性，特别是增加了介质Lewis酸性位点，有利于有效地将臭氧分解成活性氧。 γ-Fe-Ti-Al ₂ O ₃催化剂(Al/Fe=25、Al/Ti=75)提高了含溴水臭氧氧化中布洛芬的去除率，有效阻止了溴酸盐的生成。反应60 min后,TOC去除率从γ-Al ₂ O ₃ /O ₃的54%提高到γ-Fe-Ti-Al ₂ O ₃ /O ₃的86%,而单独臭氧化的只有13%。 电子顺磁共振（EPR）谱显示羟基和超氧自由基是活性氧，有利于有机质的矿化。 Fe ²⁺离子的捕获实验证实，Fe ²⁺离子与Fe ³⁺离子的电子循环有利于阻断溴化物的形成。布洛芬和腐植酸的添加可以增强γ-Fe-Ti-Al ₂ O ₃催化臭氧氧化过程中Fe ³⁺的还原，进一步强化对溴酸盐生成的阻断。