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脉冲电晕放电与TiO₂光催化协同体系中过氧化氢的生成及苯酚的降解

Formation of hydrogen peroxide and degradation of phenol in synergistic system of pulsed corona discharge combined with TiO2 photocatalysis.

作者信息

Wang Huijuan, Li Jie, Quan Xie, Wu Yan, Li Guofeng, Wang Fangzheng

机构信息

School of Environmental and Biological Science and Technology, Dalian University of Technology, Dalian 116024, China.

出版信息

J Hazard Mater. 2007 Mar 6;141(1):336-43. doi: 10.1016/j.jhazmat.2006.07.019. Epub 2006 Jul 15.

Abstract

In the present work, a synergistic system of pulsed corona discharge combined with TiO(2) photocatalysis has been developed to investigate the degradation rate of phenol solutions by varying experimental conditions of gas bubbling varieties (air, O(2), and Ar), solution pH values, and radical scavenger additives. The hydrogen peroxide (H(2)O(2)) concentration, which indicated the amount of hydroxyl radicals (OH) in the reaction system under different conditions of gas bubbling varieties and scavenger species, was also reviewed. The obtained results revealed that degradation efficiency of phenol could be increased by the addition of TiO(2) in pulsed discharge system. The gas of Ar and O(2) bubbled into the reaction system was found to be favorable for phenol degradation and H(2)O(2) formation. Both in air bubbling and in O(2) bubbling reaction system, the higher degradation rate of phenol occurred in the case of acidic solution. The addition of sodium carbonate or n-butanol in the solution displayed a negative effect for phenol removal, while the H(2)O(2) concentration showed different changing trend by adding different radical scavengers. The most effective degradation of the three main intermediates of catechol, 1,4-hydroquinone, and 1,4-benzoquinone formed during phenol decomposition existed in the synergistic system of pulsed corona discharge and TiO(2) photocatalysis bubbled with O(2).

摘要

在本研究中,开发了一种脉冲电晕放电与TiO₂光催化相结合的协同体系,通过改变气体鼓泡种类(空气、O₂和Ar)、溶液pH值以及自由基清除剂添加剂等实验条件,研究苯酚溶液的降解速率。还考察了在不同气体鼓泡种类和清除剂种类条件下,反应体系中表征羟基自由基(OH)量的过氧化氢(H₂O₂)浓度。所得结果表明,在脉冲放电体系中添加TiO₂可提高苯酚的降解效率。发现向反应体系中鼓入Ar和O₂气体有利于苯酚降解和H₂O₂生成。在空气鼓泡和O₂鼓泡反应体系中,酸性溶液中苯酚的降解速率较高。向溶液中添加碳酸钠或正丁醇对苯酚去除有负面影响,而添加不同自由基清除剂时H₂O₂浓度呈现不同变化趋势。在O₂鼓泡的脉冲电晕放电与TiO₂光催化协同体系中,苯酚分解过程中形成的邻苯二酚、1,4 - 对苯二酚和1,4 - 苯醌这三种主要中间体的降解效果最为显著。

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