Preparation of Ce-MnOX/γ-Al2O3 by high gravity-assisted impregnation method for efficient catalytic ozonation

催化作用 硝基苯 煅烧 X射线光电子能谱 化学 臭氧 氧气 高分辨率透射电子显微镜 氧化还原 激进的 羟基自由基 核化学 无机化学 材料科学 化学工程 有机化学 透射电子显微镜 纳米技术 工程类
作者
Shengjuan Shao,Zhixing Li,Jingwen Zhang,Kechang Gao,Youzhi Liu,Weizhou Jiao
出处
期刊:Chemical Engineering Science [Elsevier BV]
卷期号:248: 117246-117246 被引量:29
标识
DOI:10.1016/j.ces.2021.117246
摘要

In this study, Ce-MnOX/γ-Al2O3 was prepared by the facile high gravity-assisted impregnation method for catalytic ozonation of nitrobenzene, and a three-level and seven-factor orthogonal test was used to optimize the preparation parameters. The catalyst prepared by impregnating γ-Al2O3 in 0.24 M solution at a Ce/Mn molar ratio of 3:7, a rotational speed NR of 1000 rpm, a liquid flow rate QR of 80 L/h, and a calcination temperature T of 500 °C showed the best catalytic activity. The HRTEM results showed that the active components were highly dispersed on the surface of Ce-MnOX/γ-Al2O3 with wt% of Mn and Ce being 2.08 and 2.86, respectively. The catalytic performance showed that the nitrobenzene removal was accelerated in Ce-MnOX/γ-Al2O3 with the TOC removal of 98.3% within 20 min, which was superior to the single ozonation. The EPR and electrochemical analysis showed that Ce-MnOX/γ-Al2O3 had more oxygen vacancies, higher electron transfer capacity and lower charge transfer resistance, which was beneficial for the dissociation of ozone. Radical quenching results showed that ·O2− and ·OH were the main reactive oxygen species for the mineralization of nitrobenzene. Raman spectra and FT-IR analysis showed that oxygen vacancies and surface hydroxyl groups can act as the active sites for the decomposition of ozone into *O22− and *O2−. XPS analysis also indicated that the redox couples of Ce(IV)/Ce(III) and Mn(IV)/Mn(III) and oxygen vacancies had a synergistic effect on the decomposition of ozone into reactive oxygen species, thus improving the catalytic activity of Ce-MnOX/γ-Al2O3.
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