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1、 Experiments on Phenol Oxidated by Cavitating Water Jets with H2O2 A Thesis Submitted to Chongqing University in Partial Fulfillment of the Requirement for the Degree of Master of Engineering by Chengjun Supervisor: Prof. Lu Yiyu Major: Safety Technology and Engineering College of Resources and Envi
2、ronmental Science Chongqing University, Chongqing China. Nov. 2007 I摘 要 酚类物质是一种具有代表性的难降解有机污染物，它来源广、数量多、危害大，因此这种有机废水必须经过深度处理才能排放。含酚废水的处理方法可分为物化处理技术、生化处理技术以及高级氧化技术等几大类。但这些方法普遍存在处理不彻底等缺点。空化水射流能够提供高温（5000K） 、高压（1.013108Pa） ，这样的极端条件能促使水中 H2O2分解并释放OH 自由基，进而氧化降解一般处理方法难以降解的有机物。国内外已经有学者将其运用到五氯苯酚、苯、甲苯等有毒污染物的处
3、理中，但在苯酚废水处理上还有待进一步研究。 本论文分别采用单独 H2O2、单独空化水射流以及空化水射流结合 H2O2三种方法处理实验室配置的苯酚废水，考察了各种影响因素对苯酚去除率的影响情况，并利用高效液相色谱技术分析了空化水射流结合 H2O2氧化降解反应的中间产物和最终产物，揭示了空化水射流结合 H2O2降解苯酚的反应机理。同时建立了空化水射流结合 H2O2处理苯酚废水方法的动力学模型。论文的主要研究成果如下： 通过 H2O2单独氧化处理含酚废水的实验研究，得到 H2O2单独氧化处理含酚废水的优化反应条件为：pH 值 3.0，反应时间 180min，苯酚浓度 50mg/L，苯酚溶液的体积 1
4、L，H2O2浓度 300mg/L，苯酚最大去除率达到 31.7。 实验研究了空化水射流空化降解苯酚， 64L 体积质量浓度为 100mg/L 的苯酚溶液空化降解 3 小时后，苯酚的去除率只有 17。通过空化水射流/H2O2处理苯酚的实验研究， 得到 64L 不同浓度的苯酚溶液在该处理方法的优化反应条件为： pH 值3.0，H2O2浓度 300mg/L，苯酚浓度 100mg/L，围压 0.5MPa，废水循环次数 10 次，泵压 20MPa，苯酚去除率为 99.85。 通过考察自由基清除剂正丁醇的用量对苯酚的空化降解效果的影响及HPLC 分析探讨，明确了空化射流结合 H2O2降解苯酚的主要机理是羟
5、基自由基的氧化作用。具体推断出空化结合 H2O2氧化降解苯酚的机理：反应初期生成邻苯二酚、对苯二酚、苯醌，证明了羟基自由基的存在，羟基自由基和芳香族混合物的反应是羟基自由基与苯环发生亲电子加成反应；第二阶段产物是顺丁烯二酸和乙酸，它是苯环进一步氧化开环的结果。 空化和 H2O2的联合工艺存在很好的协同效应，通过实验数据分析得出其增强因子 f 高达 38.419。在实验研究的基础上建立了空化水射流/ H2O2工艺协同降解苯酚的动力学模型。 本论文的创新之处在于首次将空化水射流产生的空化效应结合 H2O2处理苯酚废水，揭示了空化水射流/H2O2协同降解苯酚的机理，并建立了其动力学模型。这II为焦化
6、废水等有机废水的处理提供了理论依据和实践指导。 关键词关键词：空化效应，苯酚，H2O2，OH 自由基，动力学IIIABSTRACT Phenolic contamination is a sort of representative organic pollutants which are difficult to be degraded. The numerous amount of phenolic contamination is doing great harm to the environment and can be widely found in industrial waste
7、 water. So it must be discharged with an adequate treatment. The disposal methods of phenolic waste water include physical chemistry technology, biology and advanced oxidation technology, etc. However, these methods all have some shortcomings, for instance, treatment is not thorough. High presssure
8、and high temperature could be produced after the crumble of cavitation bubble, which could impel the H2O2 in the solution to decompose into OH and degradation of organic contamination. Some scholars have applied it to the purification of some wastewater such as PCP, benzene and toluene, but further
9、research needs to be carried out on phenolic waste water with cavitation technology. This paper adopts three ways to deal with phenolic waste water and explores each kind of effecting effect on removal of phenol, these three ways are the technology of H2O2 oxidative degradation, the technology of ca
10、vitating water jets and the technology of H2O2 oxidative degradation combined with cavitating water jets. The intermediates and by- products of the technology of H2O2 oxidative degradation combined with cavitating water jets on phenol were analyzed with HPLC and the mechanism of reaction also has be
11、en confirmed. Meanwhile the dynamical model of the technology of H2O2 oxidative degradation combined with cavitating water jets has been deduced. The main contents are as follows: Through the laboratorial study on the technology of H2O2 oxidative degradation of phenolic water, the optimal reaction c
12、ondition was concluded: investigated pH 3.0, reaction time 180min, initial phenol concentration 50/mg L, phenol volume 1L, initial concentration of H2O2 300/mg L , under this optimal reaction condition, most 31.7% of phenol can be removed. The technology of cavitating water jets was adopted to deal
13、with phenol. Its volume and concentration were 64Land 100/mg L , the removal of phenol was about 17% after 3 hours reaction. Through the laboratorial study on the technology of H2O2 oxidative degradation combined with cavitating water jets on phenol, the optimal cavitation condition was obtained: in
14、vestigated pH 3.0, initial concentration of H2O2 300/mg L , initial phenol concentration 100/mg L , confining pressure 0.5MPa, IVcavitation time 12times, pumping pressure 20Mpa, under this optimal cavitation condition, most 99.85% of phenol can be removed. Through examing the influence of dosage of
15、OH radical scavenger to degradation effect of phenol, the mechanism of cavitating degradation of phenol is oxidizing of OH. And the mechanism of reaction of the technology of H2O2 oxidative degradation combined with cavitating water jets on phenol also has been confirmed by HPLC. The first step, cat
16、echol, hydroquinone and p- benzoquinone were produed which confirmed the existence of OH. The second step, maleic acid and acetic acid were produed which was the result of phenyls oxidation . Synergetic effect of cavitation and H2O2 has appeared in the technology of H2O2 oxidative degradation combined with cavitating water jets on phenol. The promoted factor for phenol degradation rate constant is found to be at about 38.419. A simplified mechanistic model f
