除草剂2，4-D的O_3、O_3/H_2O_2高级氧化技术研究
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摘要
农药污染成为近年来水环境保护领域的研究热点,苯氧羧酸类除草剂2,4-D是一种使用地域较广应用时间较长的农药,为潜在致癌物,其氯代中间产物毒性较高,可污染水体,对自然环境和人类健康造成威胁。本文主要采用臭氧化、臭氧/过氧化氢高级氧化技术,选择2,4-D为模型污染物配制模拟废水,进行动力学、机理研究,关注水质特性对2,4-D的O_3、O_3/H_2O_2氧化降解的影响,同时初步探讨臭氧/超声波联合降解2,4-D,进行臭氧化高级氧化技术的基础研究。
对2,4-D的O_3、O_3/H_2O_2氧化过程进行影响因素分析,考察反应温度、溶液pH值、2,4-D初始浓度、气体流量、H_2O_2投加量等因素对降解效果的影响,探讨较合适的条件,考察O_3和H_2O_2之间的协同作用,比较O_3、O_3/H_2O_2氧化的效果。结果表明反应温度、溶液pH值、H_2O_2投加量影响较大,气体流量影响最小,随着温度升高、pH值升高、气体流量增大、2,4-D初始浓度降低、H_2O_2投加量增大,2,4-D降解速率提高。O_3/H_2O_2体系比O_3体系稳定,O_3和H_2O_2之间具有协同作用,H_2O_2可促进O_3分解产生·OH,反应增快,降解时间缩短,反应条件温和,易于操作和改进,降低操作费用。因此O_3/H_2O_2体系更为经济有效,对降解2,4-D等有机物具有良好的运用前景,更具实用价值。
对臭氧分子直接氧化2,4-D动力学进行考察,2,4-D是可解离有机物,水溶液里呈现解离态和分子态两种,解离态的反应速率常数比分子态高,因此基于溶液中有机物解离程度,涵盖有机物的解离态、分子态反应的直接氧化动力学模型能比较好的模拟实验情况。进行2,4-D的O_3、O_3/H_2O_2氧化反应动力学研究,2,4-D降解符合拟一级动力学,有机物降解主要是羟基自由基间接氧化,在拟一级动力学反应速率常数基础上建立总动力学模型,适合于2,4-D实际氧化过程的预测。
研究2,4-D的O_3、O_3/H_2O_2氧化降解机理,对反应过程中的羟基自由基浓度和作用进行分析,结果表明2,4-D降解主要是羟基自由基起主导作用,O_3/H_2O_2体系产生的羟基自由基比O_3体系多。借助GC-MS、HPLC、IC等分析手段,测定2,4-D降解中间产物,经过合理简化和假设,跟踪反应时间内2,4-D降解的主要中间产物类的浓度变化和动力学趋势,提出2,4-D分解为含氯有机物、无氯芳香族化合物、小分子有机酸等几类中间产物的氧化反应模式及脱氯模型,研究结果表明较为复杂的交叉式降解路径能更好的说明试验结果。在单独O_3过程中可观察到有H_2O_2产生,在O_3/H_2O_2体系里则伴随H_2O_2产生和分解的过程,考察H_2O_2产生动力学模型,可以借此认识H_2O_2在O_3、O_3/H_2O_2氧化中的作用。
The treatment of pesticide pollutants is one of the hotspots in water environmental protection. 2,4-dichlorophenoxyacetic acid, a chlorophenoxy herbicides, is the most widely used herbicide worldwide due to its low cost and high effectiveness. In recent years, 2,4-D has become one of the most common surface and groundwater pollutants. The World Health Organization (WHO) considers chlorophenoxy herbicides, including 2,4-D, to be possible human carcinogens. The degradation of 2,4-D using O_3 and O_3/H_2O_2 advanced oxidation processes have been studied in this paper. The mathematical model of reaction kinetics and degradation mechanisms are derived and verified by the experiment. The effect of water qualities on 2,4-D degradation is investigated. The elementary study of 2,4-D degradation using O3/US combined technology is also carried out and the results are shown to be useful in the future research.Firstly, the influential factors such as temperature, pH levels, 2,4-D initial concentration, gas flow rate and hydrogen peroxide dose are investigated in order to find out felicity conditions in O_3 or O_3/H_2O_2 processes. Two treatments (O_3 and O_3/H_2O_2) are compared in the case of reaction efficiency which depends on the experimental parameters. The synergetic effects in O_3 and H_2O_2 in O_3/H_2O_2 combined technology are investigated. The results show that: 1) Temperature is the key factor of removal rate; 2) pH strongly affects the degradation process, and 3) Gas flow has very little influence on the efficiency of processes. Effectiveness of O3/H2O2 oxidation greatly depends on the H_2O_2 dosage. The degradation rate of 2,4-D increases with the increment of temperature, pH value, and hydrogen peroxide dose. The degradation efficiency is enhanced when 2,4-D initial concentration is decreased. Gas flow rate has both positive and negative influence on reaction; therefore, its overall effect is not evident. Compared with O3 process, O3/H2O2 greatly increases the removal efficiency of 2,4-D. The synergy of O3 and H_2O_2 is proved by the experiment. Hydrogen peroxide is the initiator of ozone decomposition chain reaction to generate hydroxyl radical. Hence, greater amounts of hydroxyl radicals are generated by the O_3/H_2O_2 system than ozonation alone. O_3/H_2O_2 has more advantages such as excellent degradation effectiveness, faster removal rate, more moderate conditions and lower operating cost than O3 system. O_3/H_2O_2 technology is an excellent advanced oxidation process in removal of 2,4-dichlorophenoxyacetic acid, and appeared to be more applicable for the treatment of wastewater.Secondly, the reaction kinetics of O3 and O_3/H_2O_2 processes are studied. This includes the kinetics of direct oxidation with ozone molecule and indirect oxidation with hydroxyl radical. The direct oxidation process is performed using radical scavenger to inhibit indirect oxidation. 2,4-D dissolved in water is dissociated to deprotonized and protonated species. The results show that reaction rate of dissociated species is fast than that of deprotonized species. It is confirmed through experiment that the relation of second-order rate constants is dependent on the degree of dissociation. A direct oxidation model in view of dissociation is proposed to predict 2,4-D degradation and proved to be agreeable to the simulated degradation. The overall degradation of 2,4-D follows the pseudo-first-order reaction. It has been found that the indirect oxidation of hydroxyl radical is dominant in 2,4-D degradation. Furthermore, the proposed overall kinetics model based on the observed psudo-fisrt-order kinetics is applied to
practical operation, and verified by the experimental results. It is shown that the model is well constructed.In order to have a better understanding of the oxidation process, the degradation mechanism is studied for 2,4-D with ozone and ozone/hydrogen peroxide. The dominant active species is identified to be hydroxyl radical and the hydroxyl radical is determined. The results show that the radical plays the key role in 2,4-D degr
对2,4-D的O_3、O_3/H_2O_2氧化过程进行影响因素分析,考察反应温度、溶液pH值、2,4-D初始浓度、气体流量、H_2O_2投加量等因素对降解效果的影响,探讨较合适的条件,考察O_3和H_2O_2之间的协同作用,比较O_3、O_3/H_2O_2氧化的效果。结果表明反应温度、溶液pH值、H_2O_2投加量影响较大,气体流量影响最小,随着温度升高、pH值升高、气体流量增大、2,4-D初始浓度降低、H_2O_2投加量增大,2,4-D降解速率提高。O_3/H_2O_2体系比O_3体系稳定,O_3和H_2O_2之间具有协同作用,H_2O_2可促进O_3分解产生·OH,反应增快,降解时间缩短,反应条件温和,易于操作和改进,降低操作费用。因此O_3/H_2O_2体系更为经济有效,对降解2,4-D等有机物具有良好的运用前景,更具实用价值。
对臭氧分子直接氧化2,4-D动力学进行考察,2,4-D是可解离有机物,水溶液里呈现解离态和分子态两种,解离态的反应速率常数比分子态高,因此基于溶液中有机物解离程度,涵盖有机物的解离态、分子态反应的直接氧化动力学模型能比较好的模拟实验情况。进行2,4-D的O_3、O_3/H_2O_2氧化反应动力学研究,2,4-D降解符合拟一级动力学,有机物降解主要是羟基自由基间接氧化,在拟一级动力学反应速率常数基础上建立总动力学模型,适合于2,4-D实际氧化过程的预测。
研究2,4-D的O_3、O_3/H_2O_2氧化降解机理,对反应过程中的羟基自由基浓度和作用进行分析,结果表明2,4-D降解主要是羟基自由基起主导作用,O_3/H_2O_2体系产生的羟基自由基比O_3体系多。借助GC-MS、HPLC、IC等分析手段,测定2,4-D降解中间产物,经过合理简化和假设,跟踪反应时间内2,4-D降解的主要中间产物类的浓度变化和动力学趋势,提出2,4-D分解为含氯有机物、无氯芳香族化合物、小分子有机酸等几类中间产物的氧化反应模式及脱氯模型,研究结果表明较为复杂的交叉式降解路径能更好的说明试验结果。在单独O_3过程中可观察到有H_2O_2产生,在O_3/H_2O_2体系里则伴随H_2O_2产生和分解的过程,考察H_2O_2产生动力学模型,可以借此认识H_2O_2在O_3、O_3/H_2O_2氧化中的作用。
The treatment of pesticide pollutants is one of the hotspots in water environmental protection. 2,4-dichlorophenoxyacetic acid, a chlorophenoxy herbicides, is the most widely used herbicide worldwide due to its low cost and high effectiveness. In recent years, 2,4-D has become one of the most common surface and groundwater pollutants. The World Health Organization (WHO) considers chlorophenoxy herbicides, including 2,4-D, to be possible human carcinogens. The degradation of 2,4-D using O_3 and O_3/H_2O_2 advanced oxidation processes have been studied in this paper. The mathematical model of reaction kinetics and degradation mechanisms are derived and verified by the experiment. The effect of water qualities on 2,4-D degradation is investigated. The elementary study of 2,4-D degradation using O3/US combined technology is also carried out and the results are shown to be useful in the future research.Firstly, the influential factors such as temperature, pH levels, 2,4-D initial concentration, gas flow rate and hydrogen peroxide dose are investigated in order to find out felicity conditions in O_3 or O_3/H_2O_2 processes. Two treatments (O_3 and O_3/H_2O_2) are compared in the case of reaction efficiency which depends on the experimental parameters. The synergetic effects in O_3 and H_2O_2 in O_3/H_2O_2 combined technology are investigated. The results show that: 1) Temperature is the key factor of removal rate; 2) pH strongly affects the degradation process, and 3) Gas flow has very little influence on the efficiency of processes. Effectiveness of O3/H2O2 oxidation greatly depends on the H_2O_2 dosage. The degradation rate of 2,4-D increases with the increment of temperature, pH value, and hydrogen peroxide dose. The degradation efficiency is enhanced when 2,4-D initial concentration is decreased. Gas flow rate has both positive and negative influence on reaction; therefore, its overall effect is not evident. Compared with O3 process, O3/H2O2 greatly increases the removal efficiency of 2,4-D. The synergy of O3 and H_2O_2 is proved by the experiment. Hydrogen peroxide is the initiator of ozone decomposition chain reaction to generate hydroxyl radical. Hence, greater amounts of hydroxyl radicals are generated by the O_3/H_2O_2 system than ozonation alone. O_3/H_2O_2 has more advantages such as excellent degradation effectiveness, faster removal rate, more moderate conditions and lower operating cost than O3 system. O_3/H_2O_2 technology is an excellent advanced oxidation process in removal of 2,4-dichlorophenoxyacetic acid, and appeared to be more applicable for the treatment of wastewater.Secondly, the reaction kinetics of O3 and O_3/H_2O_2 processes are studied. This includes the kinetics of direct oxidation with ozone molecule and indirect oxidation with hydroxyl radical. The direct oxidation process is performed using radical scavenger to inhibit indirect oxidation. 2,4-D dissolved in water is dissociated to deprotonized and protonated species. The results show that reaction rate of dissociated species is fast than that of deprotonized species. It is confirmed through experiment that the relation of second-order rate constants is dependent on the degree of dissociation. A direct oxidation model in view of dissociation is proposed to predict 2,4-D degradation and proved to be agreeable to the simulated degradation. The overall degradation of 2,4-D follows the pseudo-first-order reaction. It has been found that the indirect oxidation of hydroxyl radical is dominant in 2,4-D degradation. Furthermore, the proposed overall kinetics model based on the observed psudo-fisrt-order kinetics is applied to
practical operation, and verified by the experimental results. It is shown that the model is well constructed.In order to have a better understanding of the oxidation process, the degradation mechanism is studied for 2,4-D with ozone and ozone/hydrogen peroxide. The dominant active species is identified to be hydroxyl radical and the hydroxyl radical is determined. The results show that the radical plays the key role in 2,4-D degr
引文
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