光催化降解五氯苯酚过程及数值模拟研究
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摘要
五氯苯酚是一种典型的有机氯农药,属于持久性有机污染物,对人类和环境具有很大的危害,对五氯苯酚处理技术的研究一直是国际关注的热点。本文采用了光催化降解技术来处理废水中的五氯苯酚,从光催化降解影响因素、降解过程分析以及工艺开发和过程数值模拟等方面进行了系统的研究。
通过五氯苯酚在催化剂表面吸附等温线的测定,得到五氯苯酚在催化剂表面的吸附符合Langmuir吸附方程并获得相应吸附特性参数;推导得到了低浓度时五氯苯酚光催化降解的一级动力学方程;通过对五氯苯酚光催化降解过程的研究,检测到三种五氯苯酚光催化降解的中间体,分别为2,3,4,5-四氯酚、2,3,4,6-四氯酚和2,5-二氯酚。
考察了溶液的pH值、催化剂投加量、紫外灯光强、曝气流速和过硫酸钾投加量对光催化降解五氯苯酚的影响进行研究,发现在光催化降解水中五氯苯酚过程中,溶液pH值越大越利于降解反应进行,紫外灯光强越大降解越快,而曝气流速、催化剂投加量和过硫酸钾投加量分别存在较优值。通过TOC的检测和亚甲基兰的退色反应验证了超声波对光催化降解五氯苯酚有明显的协同促进作用。
将超声、光催化和微滤膜有机结合,开发出新型的膜外置式超声协同光催化反应器,并利用响应面实验设计方法获得应用该反应器光催化降解五氯苯酚在TiO_2投加量0.97g,气体流速0.19m~3·h~(-1),K_2S_2O_8投加量17.00mg的操作条件下降解效率最高,降解率可达98.6%。
分析光催化降解五氯苯酚反应所具有的动力学特点,结合反应速率表达式的分析,采用计算流体力学的方法对该光催化反应进行数值模拟,并利用实验数据对模拟结果的可信度进行了验证。在此基础上选用两相流模型对反应器内流场和质量场进行模拟计算,结果得到单股上方进料的方式要优于单股下方进料的方式;单股倾斜进料时,60°夹角进料的方式最佳。
Pentachlorophenol (PCP) is a typical organic chloric pesticide, which is one of the most persistent organic pollutants. It is harmful to human and the environment. The research on reducing and controlling pollutions caused by PCP has attracted wide interests in the field of chemical engineering internationally. This study focuses on the photocatalytic degradation of pentachlorophenol and the effects of photocatalytic degradation, process analysis, technique development and mathematic simulation have been investtigated.
The adsorption characteristics of PCP on the surface of catalyst were determined from the adsorption isotherm experiments. The results are used to fit the absorption parameters of the Langmuir model. The kinetic equation of the photocatalytic degradation of pentachlorophenol at lower concentration, which was said as L-H equtions, has been presented. From the study of PCP’s photo catalytic degradation process, three intermediate were detected: 2,3,4,5-tetrachlorophenol, 2,3,4,6- tetrachlorophenol and 2,5- dichlorophenol.
The effects of of pH of the solution, quantity of catalyst, light intensity, sparging rate and dosage of potassium persulfate on the photocatalytic degradation process of PCP have been investigated. The results showed that degradation rate could be accelerated by a higher pH or a more powerful light intensity, but the quantity of catalyst, sparging rate and dosage of potassium persulfate exhibited optimal values respectively. The synergistic effect of ultrasonic to photocatalytic degradation process of PCP has been proved by mesurement of TOC and the experiments of discorloring of methylene blue.
Ultrasonic, photocatalysis and membrane were combined to develop a self-style recirculated membrane ultrasonica assisted photocatalytic reactor. With the response surface method (RSM), the optimal operationing conditions of this reactor were obtained: 0.97 g of TiO_2, 0.19m~3·h~(-1) of sparging rate, 17.00 mg dosage of K_2S_2O_8, and 98.6% degradation rate.
Based on the analysis of kinetic characteristics of photocatalytic degradation of PCP and the expressions of reactive equations, computational fluid dynamics simulations were done to study this photocatalytic degradation process. The simulation results agree well with the experimental data.. At last, the model of two phases was used to simulate the hydraulics and concentration field. The results showed that top inlet was better than inferior inlet, and 60°was the better choice in one inclined inlet.
通过五氯苯酚在催化剂表面吸附等温线的测定,得到五氯苯酚在催化剂表面的吸附符合Langmuir吸附方程并获得相应吸附特性参数;推导得到了低浓度时五氯苯酚光催化降解的一级动力学方程;通过对五氯苯酚光催化降解过程的研究,检测到三种五氯苯酚光催化降解的中间体,分别为2,3,4,5-四氯酚、2,3,4,6-四氯酚和2,5-二氯酚。
考察了溶液的pH值、催化剂投加量、紫外灯光强、曝气流速和过硫酸钾投加量对光催化降解五氯苯酚的影响进行研究,发现在光催化降解水中五氯苯酚过程中,溶液pH值越大越利于降解反应进行,紫外灯光强越大降解越快,而曝气流速、催化剂投加量和过硫酸钾投加量分别存在较优值。通过TOC的检测和亚甲基兰的退色反应验证了超声波对光催化降解五氯苯酚有明显的协同促进作用。
将超声、光催化和微滤膜有机结合,开发出新型的膜外置式超声协同光催化反应器,并利用响应面实验设计方法获得应用该反应器光催化降解五氯苯酚在TiO_2投加量0.97g,气体流速0.19m~3·h~(-1),K_2S_2O_8投加量17.00mg的操作条件下降解效率最高,降解率可达98.6%。
分析光催化降解五氯苯酚反应所具有的动力学特点,结合反应速率表达式的分析,采用计算流体力学的方法对该光催化反应进行数值模拟,并利用实验数据对模拟结果的可信度进行了验证。在此基础上选用两相流模型对反应器内流场和质量场进行模拟计算,结果得到单股上方进料的方式要优于单股下方进料的方式;单股倾斜进料时,60°夹角进料的方式最佳。
Pentachlorophenol (PCP) is a typical organic chloric pesticide, which is one of the most persistent organic pollutants. It is harmful to human and the environment. The research on reducing and controlling pollutions caused by PCP has attracted wide interests in the field of chemical engineering internationally. This study focuses on the photocatalytic degradation of pentachlorophenol and the effects of photocatalytic degradation, process analysis, technique development and mathematic simulation have been investtigated.
The adsorption characteristics of PCP on the surface of catalyst were determined from the adsorption isotherm experiments. The results are used to fit the absorption parameters of the Langmuir model. The kinetic equation of the photocatalytic degradation of pentachlorophenol at lower concentration, which was said as L-H equtions, has been presented. From the study of PCP’s photo catalytic degradation process, three intermediate were detected: 2,3,4,5-tetrachlorophenol, 2,3,4,6- tetrachlorophenol and 2,5- dichlorophenol.
The effects of of pH of the solution, quantity of catalyst, light intensity, sparging rate and dosage of potassium persulfate on the photocatalytic degradation process of PCP have been investigated. The results showed that degradation rate could be accelerated by a higher pH or a more powerful light intensity, but the quantity of catalyst, sparging rate and dosage of potassium persulfate exhibited optimal values respectively. The synergistic effect of ultrasonic to photocatalytic degradation process of PCP has been proved by mesurement of TOC and the experiments of discorloring of methylene blue.
Ultrasonic, photocatalysis and membrane were combined to develop a self-style recirculated membrane ultrasonica assisted photocatalytic reactor. With the response surface method (RSM), the optimal operationing conditions of this reactor were obtained: 0.97 g of TiO_2, 0.19m~3·h~(-1) of sparging rate, 17.00 mg dosage of K_2S_2O_8, and 98.6% degradation rate.
Based on the analysis of kinetic characteristics of photocatalytic degradation of PCP and the expressions of reactive equations, computational fluid dynamics simulations were done to study this photocatalytic degradation process. The simulation results agree well with the experimental data.. At last, the model of two phases was used to simulate the hydraulics and concentration field. The results showed that top inlet was better than inferior inlet, and 60°was the better choice in one inclined inlet.
引文
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