典型持久性有机污染物在城市污水处理过程中的迁移转化规律研究
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摘要
持久性有机污染物(POPs)作为具有高毒性、难降解性、生物蓄积性的有毒有害物质对生态环境、生物体及人类健康具有严重危害。随着现代石化产业的迅猛发展,石化产品的不完全燃烧、垃圾燃烧和塑料产品的大量使用,使POPs对环境的危害日益严重,而城市污水作为人们生活和生产过程中污染物排出(或排泄)的载体,集中了大量包括POPs在内的各类污染物质。在城市污水再生利用已成为必然趋势的情况下,回用水中可能残余的各种有毒有害物质尤其是POPs的健康和环境影响问题日益备受关注。因此,有必要系统性研究POPs在城市污水中POPs的存在水平以及在常规污水处理中的迁移转化规律。
本课题是国家自然科学基金重点项目(50838005)的部分研究内容,选择4类POPs—多环芳烃(PAHs)、邻苯二甲酸酯(PAEs)、多氯联苯(PCBs)和有机氯农药(OCPs)作为研究对象,针对西安市某污水处理厂的氧化沟处理工艺,开展了污水厂各阶段出水的长期水质监测,结合实验室试验,研究了典型POPs在污水二级生化处理过程中的迁移转化规律,建立了典型POPs去除的数学模型,通过模拟计算和理论分析,论述了POPs的去除作用机理。论文的主要工作和成果如下:
(1)优化了污水中PAHs、PAEs、PCBs、OCPs的分析检测方法,通过GC-MS对4类POPs的44种标准样品进行了定性分析,确立了每类POPs的最佳色谱分离和质谱检测条件:对于16种PAHs和6种PAEs,宜通过GC-FID检测进行外标法定量分析;对于6种PCBs和16种OCPs,宜通过GC-ECD检测进行外标法定量分析。优化的GC-FID和GC-ECD检测法具有检测时间短(34.47min和26.62min)、色谱图分离效果好的特点。通过各种试样前处理条件比较,确立了实现4类POPs同时回收的固相萃取法,在优化的条件下,4类POPs的回收率均可达到70%以上。
(2)针对西安市某污水厂的氧化沟处理工艺,进行了为期1年的各工艺段出水的水质监测,结果表明,在进厂污水中主要监测到8种PAHs、5种PAEs、5种PCBs和5种OCPs,其中,PAEs浓度最高,为10~0~10~2μg/L量级,PAHs浓度次之,为100μg/L量级及以下,而PCBs和OCPs的浓度水平则在101ng/L量级及以下。氧化沟工艺对各种POPs均有明显的去除效果,多数POPs的去除率为50%~100%,且POPs的去除主要在生化处理单元完成,沉砂池和二沉池对POPs去除的作用不明显。
(3)选择进厂污水中检出浓度较高的萘(NAPT)、菲(PHEN)、芘(PYR)等3种PAHs,邻苯二甲酸二丁酯(DBP)、邻苯二甲酸二-(2-乙基己基)酯(DEHP)等2种PAEs作为典型POPs,通过实验室试验研究了石英砂、高岭土和黄土等3种无机颗粒和实验室培养的活性污泥对典型POPs的吸附去除过程。吸附试验结果表明,无机颗粒对5种典型POPs的吸附符合Langumuir吸附等温式,且具有放热过程的特点,但吸附能力有限;而活性污泥对典型POPs的吸附符合Freundlich吸附等温式,且具有吸热过程的特点,吸附能力较无机颗粒高出1个数量级以上。无机颗粒对POPs的吸附呈单层吸附的特征,比表面积是影响其吸附能力的重要因素;而活性污泥的网状絮体构造使其对POPs的吸附具有多层吸附的特征,从而吸附能力增大。对于作为吸附质的典型POPs而言,其辛醇-水分配系数(lgk_(ow))直接影响其在颗粒上的吸附,lgk_(ow)大的POPs易于被吸附去除。
(4)根据污水二级生化处理的工艺特点,研究了污水厂中POPs去除的挥发作用、吸附作用和生物降解作用机理,建立了三种作用的定量计算方程式。各种典型POPs在三种作用下的去除均与其分子结构和物化参数有关,其中吸附作用下的去除取决于POPs在液固两相间的分配系数Kp,它与吸附等温式的参数密切相关,通过污水处理过程物料平衡关系分析,提出了基于上述三种作用的典型POPs去除量计算数学模型。以监测的污水厂为例确定了与污水处理工艺相关的计算参数,对三种作用去除的分析计算结果表明,挥发在各种POPs去除中的作用极小,可忽略不计;不同的POPs生化降解性不同,NAPT、DBP和PHEN的生化降解去除率分别为13.7%、3.5%和1.5%,而PYR和DEHP的生化降解去除率均在0.1%以下,说明吸附是POPs去除的主要作用机理。针对吸附作用建立了基于吸附分配系数Kp的POPs吸附去除率计算模型,在以氧化沟中活性污泥作为POPs吸附主体的条件下,计算结果表明POPs吸附去除率随K_p值增大而增大,且在较高K_p值时趋于一定值。污水厂的实测结果与计算结果具有良好的吻合性。
论文的上述研究工作揭示了典型POPs在城市污水以及常规二级污水处理流程中的分布和迁移转化规律,具有重要的理论意义。
Persistent organic pollutants (POPs) constitute a class of man-made chemicals with pronounced highly toxic, persistence against chemical/biological degradation, tendency for bioaccumulation in human and animal tissues, and significant impacts on human health and the environment. With the wide development of modern petrifaction industry, impacts from POPs were seriously increased because of the incomplete and rubbish combustion of the petrifaction products and mass use for the plastic products. Thus, the domestic wastewater, as a carrier of pollutants discharge in life and production process, gathers much various pollutants including the POPs. So it is a necessary trend that the domestic wastewater would be reused as main supplement water. Further, it is paid more attention that all kinds of possible remained toxic and harmful materials, especially POPs, impact on the water environmental ecology in the reuse of domestic wastewater. And it appears essential to make sure the existence level in the municipal wastewater and the removal and transformed laws in the conventional wastewater treatment for the POPs.
The study was part of the National Natural Science Foundation of China (Grant No. 50838005), it chose 4 classes POPs as the studied objects, namely Polycyclic aromatic hydrocarbons (PAHs), phthalic acid esters (PAEs), polychlorinated biphenyls (PCBs), organic chlorinate pesticides (OCPs). For investigating the wastewater treatment plant in Xi’an by an oxidation ditch process, a long-term the effluent detection of the each phase of the WWTP was done. In addition of the experimental study on the removal mechanism, we establish a removal POPs mathematical model for the conventional secondary treatment process on the municipal wastewater on the basis of the analysis of the mechanism and material equilibrium. The model was simulated to get the ideal results by using the experimental data, the operating parameters and the typical POPs characteristic parameters. The studied conclusions deepen the understanding on the removal and transform mechanism of the POPs in the conventional secondary treatment process. Mainly results and discussions included:
(1) The detection analysis method of the PAHs, PAEs, PCBs and OCPs was optimized and perfected. The standard samples of 44 typical pollutions in the above 4 classes POPs were qualifier analyzed by using the GC-MS to optimize each GC conditions and MS conditions on the basis of the other references. Moreover, 16 PAHs and 6 PAEs using the GC-FID and 6 PCBs and 16 OCPs using the GC-ECD were quantified following the external standard calibration procedure, respectively to optimize GC and detection conditions of the 22 compounds detected on the GC-FID and GC-ECD, to get their chromatograph spectrum with the better isolation efficiency respectively in 34.47min and 26.62min. In last, through analyzing and comparing all kinds pretreatment methods for the different POPs in water, the SPE was adopted to pre-treat 4 classes POPs, and to optimize the best method condition by perfecting the recover rate in order to ensure more than 70% of the 4 class POPs.
(2) The paper detected the occurrence of the 4 classes POPs and the conventional pollution index of the effluent in each processes in the wastewater treatment plant in Xi′an. The results showed that 8 PAHs, 5 PAEs, 5 PCBs and 5 OCPs were found; among them, PAEs changed from 10~0μg/L to 10~2μg/L with highest concentration, then the concentration of PAHs was below 10~0μg/L, while PCBs and OCPs had the lowest concentration with less than 10~1ng/L. The changes of typical POPs pollutions showed that PAHs、PAEs、PCBs and OCPs were mainly removed in biochemistry unit, but less in primary settler and secondary settle.
(3) According to the wastewater level, NAPT, PHEN and PYR in NAPT, DBP and DEHP in PAEs were ensured as the typical POPs pollutions. Adopting lab-scale experiment, the study analyzed the main adsorbed removal mechanism of the typical POPs by inorganic particles quartz sands, kaolin and natural clay and activated sludge. The results indicated that the adsorption on 5 typical POPs from inorganic particles were monolayer adsorption and well followed the Langumuir equation, which was exothermic reaction. But the adsorption on 5 typical POPs from activated sludge was multilayer adsorption and may be simulated by the Freundlich equation, which was endothermic reaction. And the adsorption from activated sludge was bigger the ten orders, which was related to the adsorbents structure and physical and chemistrical features of the adsorbates; while the specific surface area of the adsorbents was one of the aspects to decide the adsorption ability, namely the adsorption would be stronger with the increase of the specific surface area. In addition, logK_(ow) of the adsorbates were direct contrasted to the adsorption, namely the adsorption would be stronger with the bigger of logK_(ow).
(4) According to the characteristics of the wastewater secondary treatment process, the paper studied the POPs removal mechanism including volatilization, adsorption and biodegradation, and established the quantify equations of three removal mechanism. The removal of typical POPs by three mechanism was related to the POPs structure and physical and chemistrical features, and the difference level of adsorption was due to the equilibrium partitioning coefficient K_p of POPs, and the K_p values could be obtained from the adsorption equations, and established the typical POPs removal mathematics model based on the three removal mechanism.The model parameters about wastewater treatment process were confirmed --take, for instance, the WWTP of Xi′an. The result showed that the POPs removal by volatilization very small, the removal can be neglected, and difference POPs had difference removal by biodegraded, the NAPT, PHEN, and PHEN removal by biodegraded respectively were 13.7%, 3.5%, and 1.5%, and PYR and DEHP with less than 0.1% removal ratio. So the adsorption became the main removal mechanism. In according to the obvious adsorption, the removal rate calculation model of POPs was established on the basis of the equilibrium partitioning coefficient K_p. Under the condition of activated sludge of the oxidation ditch as the adsorption subject, the reasonable results were obtained. The results presented that the adsorption rate of POPs increased with the K_p, and approached to a definite value at high K_p values.
The above study of paper announced the removal and transform mechanism of the typical POPs in domestic wastewater and the conventional secondary treatment process. It is very important for further study.
本课题是国家自然科学基金重点项目(50838005)的部分研究内容,选择4类POPs—多环芳烃(PAHs)、邻苯二甲酸酯(PAEs)、多氯联苯(PCBs)和有机氯农药(OCPs)作为研究对象,针对西安市某污水处理厂的氧化沟处理工艺,开展了污水厂各阶段出水的长期水质监测,结合实验室试验,研究了典型POPs在污水二级生化处理过程中的迁移转化规律,建立了典型POPs去除的数学模型,通过模拟计算和理论分析,论述了POPs的去除作用机理。论文的主要工作和成果如下:
(1)优化了污水中PAHs、PAEs、PCBs、OCPs的分析检测方法,通过GC-MS对4类POPs的44种标准样品进行了定性分析,确立了每类POPs的最佳色谱分离和质谱检测条件:对于16种PAHs和6种PAEs,宜通过GC-FID检测进行外标法定量分析;对于6种PCBs和16种OCPs,宜通过GC-ECD检测进行外标法定量分析。优化的GC-FID和GC-ECD检测法具有检测时间短(34.47min和26.62min)、色谱图分离效果好的特点。通过各种试样前处理条件比较,确立了实现4类POPs同时回收的固相萃取法,在优化的条件下,4类POPs的回收率均可达到70%以上。
(2)针对西安市某污水厂的氧化沟处理工艺,进行了为期1年的各工艺段出水的水质监测,结果表明,在进厂污水中主要监测到8种PAHs、5种PAEs、5种PCBs和5种OCPs,其中,PAEs浓度最高,为10~0~10~2μg/L量级,PAHs浓度次之,为100μg/L量级及以下,而PCBs和OCPs的浓度水平则在101ng/L量级及以下。氧化沟工艺对各种POPs均有明显的去除效果,多数POPs的去除率为50%~100%,且POPs的去除主要在生化处理单元完成,沉砂池和二沉池对POPs去除的作用不明显。
(3)选择进厂污水中检出浓度较高的萘(NAPT)、菲(PHEN)、芘(PYR)等3种PAHs,邻苯二甲酸二丁酯(DBP)、邻苯二甲酸二-(2-乙基己基)酯(DEHP)等2种PAEs作为典型POPs,通过实验室试验研究了石英砂、高岭土和黄土等3种无机颗粒和实验室培养的活性污泥对典型POPs的吸附去除过程。吸附试验结果表明,无机颗粒对5种典型POPs的吸附符合Langumuir吸附等温式,且具有放热过程的特点,但吸附能力有限;而活性污泥对典型POPs的吸附符合Freundlich吸附等温式,且具有吸热过程的特点,吸附能力较无机颗粒高出1个数量级以上。无机颗粒对POPs的吸附呈单层吸附的特征,比表面积是影响其吸附能力的重要因素;而活性污泥的网状絮体构造使其对POPs的吸附具有多层吸附的特征,从而吸附能力增大。对于作为吸附质的典型POPs而言,其辛醇-水分配系数(lgk_(ow))直接影响其在颗粒上的吸附,lgk_(ow)大的POPs易于被吸附去除。
(4)根据污水二级生化处理的工艺特点,研究了污水厂中POPs去除的挥发作用、吸附作用和生物降解作用机理,建立了三种作用的定量计算方程式。各种典型POPs在三种作用下的去除均与其分子结构和物化参数有关,其中吸附作用下的去除取决于POPs在液固两相间的分配系数Kp,它与吸附等温式的参数密切相关,通过污水处理过程物料平衡关系分析,提出了基于上述三种作用的典型POPs去除量计算数学模型。以监测的污水厂为例确定了与污水处理工艺相关的计算参数,对三种作用去除的分析计算结果表明,挥发在各种POPs去除中的作用极小,可忽略不计;不同的POPs生化降解性不同,NAPT、DBP和PHEN的生化降解去除率分别为13.7%、3.5%和1.5%,而PYR和DEHP的生化降解去除率均在0.1%以下,说明吸附是POPs去除的主要作用机理。针对吸附作用建立了基于吸附分配系数Kp的POPs吸附去除率计算模型,在以氧化沟中活性污泥作为POPs吸附主体的条件下,计算结果表明POPs吸附去除率随K_p值增大而增大,且在较高K_p值时趋于一定值。污水厂的实测结果与计算结果具有良好的吻合性。
论文的上述研究工作揭示了典型POPs在城市污水以及常规二级污水处理流程中的分布和迁移转化规律,具有重要的理论意义。
Persistent organic pollutants (POPs) constitute a class of man-made chemicals with pronounced highly toxic, persistence against chemical/biological degradation, tendency for bioaccumulation in human and animal tissues, and significant impacts on human health and the environment. With the wide development of modern petrifaction industry, impacts from POPs were seriously increased because of the incomplete and rubbish combustion of the petrifaction products and mass use for the plastic products. Thus, the domestic wastewater, as a carrier of pollutants discharge in life and production process, gathers much various pollutants including the POPs. So it is a necessary trend that the domestic wastewater would be reused as main supplement water. Further, it is paid more attention that all kinds of possible remained toxic and harmful materials, especially POPs, impact on the water environmental ecology in the reuse of domestic wastewater. And it appears essential to make sure the existence level in the municipal wastewater and the removal and transformed laws in the conventional wastewater treatment for the POPs.
The study was part of the National Natural Science Foundation of China (Grant No. 50838005), it chose 4 classes POPs as the studied objects, namely Polycyclic aromatic hydrocarbons (PAHs), phthalic acid esters (PAEs), polychlorinated biphenyls (PCBs), organic chlorinate pesticides (OCPs). For investigating the wastewater treatment plant in Xi’an by an oxidation ditch process, a long-term the effluent detection of the each phase of the WWTP was done. In addition of the experimental study on the removal mechanism, we establish a removal POPs mathematical model for the conventional secondary treatment process on the municipal wastewater on the basis of the analysis of the mechanism and material equilibrium. The model was simulated to get the ideal results by using the experimental data, the operating parameters and the typical POPs characteristic parameters. The studied conclusions deepen the understanding on the removal and transform mechanism of the POPs in the conventional secondary treatment process. Mainly results and discussions included:
(1) The detection analysis method of the PAHs, PAEs, PCBs and OCPs was optimized and perfected. The standard samples of 44 typical pollutions in the above 4 classes POPs were qualifier analyzed by using the GC-MS to optimize each GC conditions and MS conditions on the basis of the other references. Moreover, 16 PAHs and 6 PAEs using the GC-FID and 6 PCBs and 16 OCPs using the GC-ECD were quantified following the external standard calibration procedure, respectively to optimize GC and detection conditions of the 22 compounds detected on the GC-FID and GC-ECD, to get their chromatograph spectrum with the better isolation efficiency respectively in 34.47min and 26.62min. In last, through analyzing and comparing all kinds pretreatment methods for the different POPs in water, the SPE was adopted to pre-treat 4 classes POPs, and to optimize the best method condition by perfecting the recover rate in order to ensure more than 70% of the 4 class POPs.
(2) The paper detected the occurrence of the 4 classes POPs and the conventional pollution index of the effluent in each processes in the wastewater treatment plant in Xi′an. The results showed that 8 PAHs, 5 PAEs, 5 PCBs and 5 OCPs were found; among them, PAEs changed from 10~0μg/L to 10~2μg/L with highest concentration, then the concentration of PAHs was below 10~0μg/L, while PCBs and OCPs had the lowest concentration with less than 10~1ng/L. The changes of typical POPs pollutions showed that PAHs、PAEs、PCBs and OCPs were mainly removed in biochemistry unit, but less in primary settler and secondary settle.
(3) According to the wastewater level, NAPT, PHEN and PYR in NAPT, DBP and DEHP in PAEs were ensured as the typical POPs pollutions. Adopting lab-scale experiment, the study analyzed the main adsorbed removal mechanism of the typical POPs by inorganic particles quartz sands, kaolin and natural clay and activated sludge. The results indicated that the adsorption on 5 typical POPs from inorganic particles were monolayer adsorption and well followed the Langumuir equation, which was exothermic reaction. But the adsorption on 5 typical POPs from activated sludge was multilayer adsorption and may be simulated by the Freundlich equation, which was endothermic reaction. And the adsorption from activated sludge was bigger the ten orders, which was related to the adsorbents structure and physical and chemistrical features of the adsorbates; while the specific surface area of the adsorbents was one of the aspects to decide the adsorption ability, namely the adsorption would be stronger with the increase of the specific surface area. In addition, logK_(ow) of the adsorbates were direct contrasted to the adsorption, namely the adsorption would be stronger with the bigger of logK_(ow).
(4) According to the characteristics of the wastewater secondary treatment process, the paper studied the POPs removal mechanism including volatilization, adsorption and biodegradation, and established the quantify equations of three removal mechanism. The removal of typical POPs by three mechanism was related to the POPs structure and physical and chemistrical features, and the difference level of adsorption was due to the equilibrium partitioning coefficient K_p of POPs, and the K_p values could be obtained from the adsorption equations, and established the typical POPs removal mathematics model based on the three removal mechanism.The model parameters about wastewater treatment process were confirmed --take, for instance, the WWTP of Xi′an. The result showed that the POPs removal by volatilization very small, the removal can be neglected, and difference POPs had difference removal by biodegraded, the NAPT, PHEN, and PHEN removal by biodegraded respectively were 13.7%, 3.5%, and 1.5%, and PYR and DEHP with less than 0.1% removal ratio. So the adsorption became the main removal mechanism. In according to the obvious adsorption, the removal rate calculation model of POPs was established on the basis of the equilibrium partitioning coefficient K_p. Under the condition of activated sludge of the oxidation ditch as the adsorption subject, the reasonable results were obtained. The results presented that the adsorption rate of POPs increased with the K_p, and approached to a definite value at high K_p values.
The above study of paper announced the removal and transform mechanism of the typical POPs in domestic wastewater and the conventional secondary treatment process. It is very important for further study.
引文
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