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纳米级TiO_2/沸石/UV催化臭氧化处理水中硝基苯的研究
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摘要
目前利用沸石负载TiO_2处理硝基苯的方法主要是半导体光催化法。本文主要采用负载型催化剂TiO_2/沸石,结合紫外光和O_3,将硝基苯完全氧化降解。纳米TiO_2/沸石催化剂采用溶胶-凝胶法制备,制出的催化剂晶型易控制,适合实际工程使用。
     单独氧气的吹脱或催化剂吸附对去除硝基苯基本没有效果。通过系统分析O_3/TiO_2/沸石/UV体系降解硝基苯的影响因素,得出在一定范围内,随着进气流量的增加、温度的升高硝基苯的降解速率都会加快。O_3/TiO_2/沸石/UV降解硝基苯的反应属于一级反应,催化臭氧化反应速率与硝基苯的初始浓度无关。PH是影响臭氧氧化过程的一个重要因素,在弱碱性条件下降解硝基苯的效果最好。叔丁醇对硝基苯的降解有很强的抑制作用。TiO_2/沸石催化剂在使用10次时基本失活,对于失活的催化剂采用高温焙烧法可以再生。
     另外通过对各种体系降解硝基苯的TOC的研究发现单独臭氧对TOC的去除并没有效果,反应体系中有大量的中间产物产生。而光催化和臭氧联用时臭氧捕获了光催化过程中产生的光致电子e-,生成了更多的强氧化剂·OH,所以O_3/TiO_2/沸石/UV体系对TOC的去除效果最好。通过对O_3/TiO_2/沸石/UV体系降解TOC的影响因素分析,得出氧气进气流量、溶液pH值、催化剂投加量及温度的影响较大。
Nowadays the mostly used alternative of nitrobeneze treatment that based on TiO_2/zeolite catalyst is photocatalytic. This paper is employing ozone together with UV and in particular with a supported catalyst TiO_2/zeolite that can degradate nitrobeneze completely.The oxidation capacity and the photodegradation rate is far better than photocatalytic only. The nanoparticle TiO_2/zeolite catalyst which was suitable for pratical project use was prepared by the sol-gel process.TiO_2/zeolite catalyst was easy to control the crystal.
     From the experimental results obtained it is observed that there had no effect to removed nitrobeneze by only use oxygen or catalyst adsorption.Different experimental conditions in degradating nitrobeneze by O_3/TiO_2/zeolite/UV system have been examined,it was showed that with the increase in air flow and temperture,the degradation rate of nitrobeneze will accelerate.Catalytic ozoation reaction was first order with no respect to the initial concentration of nitrobeneze.PH is an important influencing factor which effected the ozone oxidation process,the best effect was received uder alkalescent condition.Tert-butyl alcohol on the degradation of nitrobeneze have a strong inhibitory effct. TiO_2/zeolite catalyst was deactivation after ten times using,and it can be renewable by high temperature roasting.
     From investigating various systems degradation of TOC,it is abtained that individual ozone on removing TOC had no effect , there had large number of intermediate products in the reaction system.The photocatalytic combined with ozone can capture the photo-induced electron-e- in the photocatalytic process,generating more strong oxidizer·OH, so O_3/TiO_2/zeolite/UV system on the effect of removing TOC was best.By analyzing the affcting factors on the degradation system of nitrobeneze,it was conculed that some experimental parameters, such as pH value, catalyst dosage and temperature effect strongly the reaction.
引文
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