TiO_(2)/γ-Al_(2)O_(3)催化臭氧氧化水中布洛芬

Catalytic ozonation of ibuprofen by TiO_(2)/γ-Al_(2)O_(3) in water

以葡萄糖为模板,采用蒸发诱导自组装法合成了γ-Al_(2)O_(3)介孔催化剂,以钛酸四正丁酯(TBOT)为原料制备TiO_(2)/γ-Al_(2)O_(3)催化剂,并将其用于催化臭氧氧化水中布洛芬(IBU).X射线衍射、扫描电子显微镜、氮气吸附-脱附和吡啶红外光谱表征结果表明,TiO_(2)均匀负载于γ-Al_(2)O_(3)表面,保持γ-Al_(2)O_(3)有序的介孔结构,具有较大的比表面积和更多的Lewis酸性位.不同催化剂活性评价结果表明,TiO_(2)的负载显著提高γ-Al_(2)O_(3)催化臭氧氧化水中布洛芬的活性,反应60 min,TiO_(2)/γ-Al_(2)O_(3)催化剂的TOC去除率达到80%,而γ-Al_(2)O_(3)、TiO_(2)及单独臭氧氧化过程中TOC去除率则分别达到62%、32%及26%.电子顺磁共振和原位激光显微拉曼光谱实验结果表明,Lewis酸性位为臭氧高效分解的活性位,活性原子氧和过氧物种是TiO_(2)/γ-Al_(2)O_(3)催化臭氧氧化反应的活性氧物种,有利于有机物的矿化,从而表现出最高的催化活性.重复利用实验结果表明,TiO_(2)/γ-Al_(2)O_(3)催化剂具有较长的使用寿命.

Theγ-Al_(2)O_(3) mesoporous catalyst was synthesized by evaporation-induced self-assembly method using glucose as template.TiO_(2)/γ-Al_(2)O_(3) catalyst was prepared from tetrabn-butyl titanate(TBOT)as raw material,and was used to catalytic ozonation of ibuprofen(IBU)in water.The results of X-ray diffraction,scanning electron microscopy,nitrogen adsorption-desorption and pyridine infrared spectroscopy showed that titanium dioxide was uniformly loaded on the surface ofγ-Al_(2)O_(3),maintaining the ordered mesoporous structure ofγ-Al_(2)O_(3),with larger specific surface area and more Lewis acidic sites.The evaluation results of different catalyst activities showed that TiO_(2) support significantly improved the activity ofγ-Al_(2)O_(3) catalytic ozonation of ibuprofen in water,and the TOC removal rate of TiO_(2)/γ-Al_(2)O_(3) catalyst reached 80%after 60 min reaction.The TOC removal rates ofγ-Al_(2)O_(3),TiO_(2) and ozonation alone reached 62%,32%and 26%,respectively.The results of electron paramagnetic resonance(EPR)and in-situ laser micro-Raman spectroscopy showed that Lewis acid sites were the active site for effective decomposition of ozone,while active atomic oxygen and peroxy species were the active oxygen species of TiO_(2)/γ-Al_(2)O_(3) catalytic ozonation reaction,which was conducive to the mineralization of organic matter and showed the highest catalytic activity.The reuse experiment results showed that the TiO_(2)/γ-Al_(2)O_(3) catalyst had a long service life.