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超声正交双频催化臭氧化降解水溶液中硝基苯的强化机制

Enhanced mechanism of catalytic ozonation by ultrasound with orthogonal dual frequencies for the degradation of nitrobenzene in aqueous solution.

作者信息

Zhao Lei, Ma Jun, Zhai Xuedong

机构信息

School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin 150090, People's Republic of China.

出版信息

Ultrason Sonochem. 2010 Jan;17(1):84-91. doi: 10.1016/j.ultsonch.2009.07.001. Epub 2009 Jul 14.

DOI:10.1016/j.ultsonch.2009.07.001
PMID:19666236
Abstract

The experiments have been performed with a semi-continuous batch reactor to investigate the degradation efficiency of nitrobenzene in aqueous solution by ultrasound with the different orthogonal dual frequencies catalytic ozonation. The introduction of ultrasound can enhance the degradation efficiency of nitrobenzene compared to the results obtained from the processes of ozonation alone and ultrasound alone. The degradation of nitrobenzene is found to be zero-order in the two systems of ultrasound alone, and the reactions follow the pseudo-first-order kinetic model in the processes of ozone alone and ozone/ultrasound. The investigation confirms that the degradation of nitrobenzene follows the mechanism of hydroxyl radical (()OH) oxidation, and the enhancement function is even more pronounced in the presence of ultrasound with the greater difference between the orthogonal dual frequencies due to the obvious synergetic effect between ozone and ultrasound, which increases the utilization efficiency of ozone, and accelerates the initiation of ()OH and the formation of H(2)O(2), resulting in the rapid formation of an increasing diversity of byproducts and the advancement degree of mineralization of total organic carbon (TOC). The oxidative byproducts have been, respectively identified in the different processes selected, including o, p, m-nitrophenols, phenol, malonic acid, 4-nitrocatechol, nitrate ion, maleic acid, oxalic acid, hydroquinone, p-quinone, 1,2,3-trihydroxy-5-nitrobenzene and acetic acid.

摘要

采用半连续间歇式反应器进行实验,以研究不同正交双频催化臭氧化条件下超声对水溶液中硝基苯的降解效率。与单独臭氧化和单独超声处理的结果相比,引入超声可提高硝基苯的降解效率。在单独超声的两个体系中,硝基苯的降解为零级反应,在单独臭氧和臭氧/超声过程中,反应遵循准一级动力学模型。研究证实,硝基苯的降解遵循羟基自由基(()OH)氧化机制,由于臭氧与超声之间存在明显的协同效应,在正交双频差异较大的超声存在下,增强作用更为显著,这提高了臭氧的利用效率,加速了()OH的产生和H(2)O(2)的形成,导致副产物种类迅速增加,总有机碳(TOC)矿化程度提高。在所选的不同过程中分别鉴定出了氧化副产物,包括邻、间、对硝基苯酚、苯酚、丙二酸、4-硝基邻苯二酚、硝酸根离子、马来酸、草酸、对苯二酚、对苯醌、1,2,3-三羟基-5-硝基苯和乙酸。

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