Yan Liqiang, Bing Jishuai, Wu Hecheng
School of Economics and Management, Nanjing University of Aeronautics and Astronautics, Nanjing, People's Republic of China.
Marine Resources Development Institute of Jiangsu, Jiangsu Ocean University, Lianyungang, People's Republic of China.
Environ Technol. 2021 Sep 9:1-10. doi: 10.1080/21622515.2021.1937333.
Iron and titanium doped γ-AlO (γ-Fe-Ti-AlO) 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-AlO, uniform distribution, maintain the ordered mesoporous structure of γ-AlO, with larger specific surface area. The valence of titanium coexists with Ti and Ti, and the valence of iron was Fe. Infrared spectra of chemisorbed pyridine (Py-FTIR) results showed that the doped titanium and iron into the framework position of γ-AlO 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-AlO 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-AlO/O to 86% with γ-Fe-Ti-AlO/O, 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 Fe ion confirmed that the electronic cycle of Fe ion and Fe ion was beneficial to block the formation of bromated. The addition of ibuprofen and humic acid can enhance the reduction of Fe in the catalytic ozonation of γ-Fe-Ti-AlO, which further strengthened the blocking of bromate formation.
以葡萄糖为模板,通过蒸发诱导自组装法合成了铁和钛掺杂的γ -AlO(γ-Fe-Ti-AlO)介孔催化剂,并将其应用于含溴水中布洛芬的臭氧化反应。X射线衍射(XRD)、氮吸附-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-AlO骨架中,分布均匀,保持了γ-AlO的有序介孔结构,比表面积较大。钛的价态以Ti和Ti共存,铁的价态为Fe。化学吸附吡啶的红外光谱(Py-FTIR)结果表明,掺杂到γ-AlO骨架位置的钛和铁改变了氧化铝表面的酸度,特别是增加了中等强度的路易斯酸位点,有利于臭氧有效分解为活性氧物种。γ-Fe-Ti-AlO催化剂(Al/Fe = 25,Al/Ti = 75)提高了含溴水中布洛芬臭氧化反应的去除率,并有效阻止了溴酸盐的形成。反应60分钟后,γ-Fe-Ti-AlO/O体系中总有机碳(TOC)的去除率从γ-AlO/O体系的54%提高到86%,而单独臭氧化时仅为13%。电子顺磁共振(EPR)光谱表明,羟基和超氧自由基是活性氧物种,有利于有机物的矿化。Fe离子捕获实验证实,Fe离子和Fe离子的电子循环有利于阻止溴酸盐的形成。布洛芬和腐殖酸的加入可以增强γ-Fe-Ti-AlO催化臭氧化过程中Fe的还原,进一步加强对溴酸盐形成的阻断。