污水处理系统中磺胺嘧啶和磺胺甲噁唑的优化处理研究
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摘要
抗生素的环境污染及其生态毒理效应已成为我国乃至全球所面临的重大环境问题之一。随着环境检测分析手段的快速发展和应用，给排水系统中抗生素等微污染物的残留、危害、去除机制等己逐渐引起了环境工作者和公众的广泛关注。
城市污水的再生利用是解决当前水资源日益短缺的有效途径之一。城市污水处理厂已成为抗生素药物进入环境的主要污染源之一。而现有的多数传统污水处理工艺对抗生素的去除效率不高，且去除机制存在争议。故进入水体中的抗生素成为城市污水再生利用的一个巨大挑战。因此，如何在保证现有污水厂处理工艺对常规污染物较高去除率的基础上，探讨研究一套可靠、高效、经济可行的以去除抗生素为目的的优化处理工艺已成为亟待解决的问题。
为了提高现有污水处理系统中磺胺类抗生素的去除率，本文在调查研究了泰安市两座污水处理厂各工段中SD与SMX浓度分布特征的基础上，采取传统污水处理系统SBR法和两类典型深度处理工艺优化处理人工污水中SD与SMX，系统的研究了处理工艺的影响因素和最佳工艺参数，提出了改进现有污水厂强化抗生素去除率的工艺流程。论文的主要研究内容如下：
（1）采用固相萃取—高效液相色谱法对泰安市两座污水处理厂磺胺嘧啶和磺胺甲噁唑的污染特征分析。结果表明，不同污水来源的处理厂中进水浓度不同，以生活污水为主的A厂进水浓度为165.8ng L-1和324.3ng L-1，而以工业废水为主的B厂中进水浓度分别为88.9和165.3ng L-1；处理工艺不同，去除效率不同，A厂、B厂SD与SMX去除率分别为48.3%、44.9%和39.1%、35.8%；A厂中不同工段的去除率不同，其中的好氧单元去除率最高，SD和SMX去除率为29.0%和20.6%%；污水中SD和SMX的去除机制主要是吸附到颗粒物上，浓缩污泥中SD和SMX浓度分别为135.4和285.3ng g-1。
（2）采用延长污泥龄和增加曝气时间的方法优化了SBR法去除污水中两种磺胺类抗生素工艺参数。实验结果表明，延长SBR总HRT、提高好氧时间段-厌氧时间段的比例和延长SRT有助于提高SD与SMX的去除率，当总HRT时间为480min时，SRT为25d，好氧-厌氧时间比为0.83时，SD与SMX去除率维持在48~56%、51~58%；
（3）采用Fenton试剂法、高铁酸盐法和吸附法强化了污水系统中两种抗生素的去除效率。实验结果表明，当污水量为0.4L，SD与SMX浓度为1.0mg·L-1时，采用高铁酸盐去除SD与SMX，其最佳投加量为0.15mmoL·L-1，pH为6~7，温度为25℃，反应最佳时间为10min，SD与SMX的去除率达到88.6%和88.9%；采用Fenton试剂法去除SD与SMX时，其去除率随氧化剂和催化剂投加量的增加而升高，其最佳投加量为Fe2+0.015mmoL·L-1，H2O20.2mmoL·L-1，反应初始pH为4，温度为25℃，反应最佳时间为60min，SD与SMX的去除率达到92%和99%以上；采用大孔树脂吸附法去除SD与SMX时，其最佳投加量分别为1.6g，pH为6~7，反应平衡时间为120min，吸附温度为20℃，SD与SMX的去除率达到80.8%和88.2%，SD与SMX的去除符合拟一级动力学模型；采用活性炭去除SD与SMX时，其最佳投加量为100mg，pH为6~7，反应平衡时间为180min，SD与SMX的去除率达到79.7%和91.5%，SD与SMX的去除符合拟一级动力学模型。
同时，实验结果表明，优化后的SBR工艺对常规指标可以保持原有的去除效率。深度处理法对常规指标的去除效率不高，去除率仅有10%~35%左右。在传统生物处理的污水系统中，增加深度处理法可有效去除污水中常规污染物和微量污染物。
Environmental pollution and eco-toxicological effects of antibiotics has become one of the majorenvironmental problems in China and even in the whole world. With the rapid development and applicationof environmental detection and analysis measures, the residual, hazards and removal of micro pollutantssuch as antibiotics in the drainage systems has gradually caused wide concern among the public, especiallythe environmentalist.
Recycling of urban sewage is one way of effective solutions to the current growing water scarcity. Theurban sewage treatment plant has become one of the main sources of antibiotic drugs into the environment.Because most of the existing traditional wastewater treatment process of removing antibiotics is not soeffective and the mechanism of removal is controversial, antibiotics discharged into the water have becomea great challenge to the municipal wastewater recycling. So it has become a serious problem to discuss andresearch a reliable, efficient and economically feasible treatment process aimed at removing the antibioticon the basis of higher efficiency of the existing sewage treatment plant to remove the common pollutants.
In order to improve the removal of sulfonamides in the existing wastewater treatment system,thispaper,based on investigating the concentration distribution of sulfadiazine(SD) and sulfamethoxazole(SMX)in each section of two sewage treatment plants in Tai'an City, took traditional treatment process SBR andtwo types of typical advanced treatment process to optimize the SD and SMX in artificial wastewater,studied systematically the influencing factors of treatment process and optimum parameters, and finally putforward a process of improving the removal of antibiotics in the existing wastewater treatment plants. Themain contents are as follows:
（1）Analyzed the pollution characteristics of SD and SMX in two sewage treatment plants of Tai'anCity by solid-phase extraction and high performance liquid chromatography (HPLC). The results showedthat influent concentration varies from different sources of sewage: The influent concentration of SD andSMX were165.8ng L-1and324.3ng L-1in Plant A for domestic sewage and the influent concentrationswere88.9and165.3ng L-1in Plant B for industrial wastewater; that removal rates varied from differentprocesses: the removal rates of SD and SMX in Plant A and B were48.3%、44.9%and39.1%、35.8%respectively; that the removal rates varied from different sections in Plant A, and the highest removalefficiency took place in aerobic cells, in which removal rates of SD and SMX were29.0%and20.6%%;that the removal mechanisms of SD and SMX were mainly adsorbed into particulate matter and theconcentrations of SD and SMX in concentrated sludge were135.4and285.3ng g-1.
（2） Optimized the parameters of removing two sulfa antibiotics in the SBR wastewater process byextending the sludge reaction time (SRT) and hydraulic reaction time (HRT). Experimental results showedthat extending the total HRT, improving the proportion of aerobic period-anaerobic period and extending the SRT contributed to the removal rates of SD and SMX: when the total HRT was480min, the SRT was25d, and the aerobic to anaerobic ratio was0.83, the removal rates of SD and SMX maintained at48~56%,51~58%;
(3) Strengthened the efficiency of the removal of two antibiotics in the sewage system by usingFenton reagent method, ferrate method and adsorption method. Experimental results showed that when thedischarge of sewage was0.4L and the concentration of SD and SMX was1.0mg·L-1, for the method offerrate, the optimum dosage was0.15mmoL L-1, pH was from6to7, the temperature was25℃, and thebest reaction time was10min, when the removal rates of SD and SMX reached88.6%and88.9%; for theFenton reagent method，the removal rate increased with the oxidant and catalyst dosage increased, theoptimum dosage was Fe2+=0.015mmoL L-1, H12O2=0.2mmoL L-, the initial reaction pH was4, thetemperature was25℃, the best reaction time was60min, the removal rates of SD and SMX reached92%and over99%; for the microporous resin adsorption method, the optimal dosage was1.6g, pH was from6to7, the equilibrium time was120min, absorption temperature was20℃, the removal rates of SD andSMX were80.8%and88.2%，and the removals of SD and SMX’s were in line with the first order kineticsmodel; when using activated carbon to remove SD and SMX, the optimum dosage was100mg, pH wasfrom6to7, the equilibrium time was180min., the removal rates of SD and SMX reached79.7%and91.5%and the removals of SD and SMX’s were in line with the first order kinetics model.
Meanwhile，the experimental results showed that optimized SBR technology could maintain theoriginal removal efficiency for the conventional indicators such as COD; that the advanced treatment is notso effective for the conventional indicators, and the removal rate was only about10%~35%; in sewagesystems of conventional biological treatment，increasing the depth treatment could effectively removeconventional pollutants and trace contaminants in sewage.
城市污水的再生利用是解决当前水资源日益短缺的有效途径之一。城市污水处理厂已成为抗生素药物进入环境的主要污染源之一。而现有的多数传统污水处理工艺对抗生素的去除效率不高，且去除机制存在争议。故进入水体中的抗生素成为城市污水再生利用的一个巨大挑战。因此，如何在保证现有污水厂处理工艺对常规污染物较高去除率的基础上，探讨研究一套可靠、高效、经济可行的以去除抗生素为目的的优化处理工艺已成为亟待解决的问题。
为了提高现有污水处理系统中磺胺类抗生素的去除率，本文在调查研究了泰安市两座污水处理厂各工段中SD与SMX浓度分布特征的基础上，采取传统污水处理系统SBR法和两类典型深度处理工艺优化处理人工污水中SD与SMX，系统的研究了处理工艺的影响因素和最佳工艺参数，提出了改进现有污水厂强化抗生素去除率的工艺流程。论文的主要研究内容如下：
（1）采用固相萃取—高效液相色谱法对泰安市两座污水处理厂磺胺嘧啶和磺胺甲噁唑的污染特征分析。结果表明，不同污水来源的处理厂中进水浓度不同，以生活污水为主的A厂进水浓度为165.8ng L-1和324.3ng L-1，而以工业废水为主的B厂中进水浓度分别为88.9和165.3ng L-1；处理工艺不同，去除效率不同，A厂、B厂SD与SMX去除率分别为48.3%、44.9%和39.1%、35.8%；A厂中不同工段的去除率不同，其中的好氧单元去除率最高，SD和SMX去除率为29.0%和20.6%%；污水中SD和SMX的去除机制主要是吸附到颗粒物上，浓缩污泥中SD和SMX浓度分别为135.4和285.3ng g-1。
（2）采用延长污泥龄和增加曝气时间的方法优化了SBR法去除污水中两种磺胺类抗生素工艺参数。实验结果表明，延长SBR总HRT、提高好氧时间段-厌氧时间段的比例和延长SRT有助于提高SD与SMX的去除率，当总HRT时间为480min时，SRT为25d，好氧-厌氧时间比为0.83时，SD与SMX去除率维持在48~56%、51~58%；
（3）采用Fenton试剂法、高铁酸盐法和吸附法强化了污水系统中两种抗生素的去除效率。实验结果表明，当污水量为0.4L，SD与SMX浓度为1.0mg·L-1时，采用高铁酸盐去除SD与SMX，其最佳投加量为0.15mmoL·L-1，pH为6~7，温度为25℃，反应最佳时间为10min，SD与SMX的去除率达到88.6%和88.9%；采用Fenton试剂法去除SD与SMX时，其去除率随氧化剂和催化剂投加量的增加而升高，其最佳投加量为Fe2+0.015mmoL·L-1，H2O20.2mmoL·L-1，反应初始pH为4，温度为25℃，反应最佳时间为60min，SD与SMX的去除率达到92%和99%以上；采用大孔树脂吸附法去除SD与SMX时，其最佳投加量分别为1.6g，pH为6~7，反应平衡时间为120min，吸附温度为20℃，SD与SMX的去除率达到80.8%和88.2%，SD与SMX的去除符合拟一级动力学模型；采用活性炭去除SD与SMX时，其最佳投加量为100mg，pH为6~7，反应平衡时间为180min，SD与SMX的去除率达到79.7%和91.5%，SD与SMX的去除符合拟一级动力学模型。
同时，实验结果表明，优化后的SBR工艺对常规指标可以保持原有的去除效率。深度处理法对常规指标的去除效率不高，去除率仅有10%~35%左右。在传统生物处理的污水系统中，增加深度处理法可有效去除污水中常规污染物和微量污染物。
Environmental pollution and eco-toxicological effects of antibiotics has become one of the majorenvironmental problems in China and even in the whole world. With the rapid development and applicationof environmental detection and analysis measures, the residual, hazards and removal of micro pollutantssuch as antibiotics in the drainage systems has gradually caused wide concern among the public, especiallythe environmentalist.
Recycling of urban sewage is one way of effective solutions to the current growing water scarcity. Theurban sewage treatment plant has become one of the main sources of antibiotic drugs into the environment.Because most of the existing traditional wastewater treatment process of removing antibiotics is not soeffective and the mechanism of removal is controversial, antibiotics discharged into the water have becomea great challenge to the municipal wastewater recycling. So it has become a serious problem to discuss andresearch a reliable, efficient and economically feasible treatment process aimed at removing the antibioticon the basis of higher efficiency of the existing sewage treatment plant to remove the common pollutants.
In order to improve the removal of sulfonamides in the existing wastewater treatment system,thispaper,based on investigating the concentration distribution of sulfadiazine(SD) and sulfamethoxazole(SMX)in each section of two sewage treatment plants in Tai'an City, took traditional treatment process SBR andtwo types of typical advanced treatment process to optimize the SD and SMX in artificial wastewater,studied systematically the influencing factors of treatment process and optimum parameters, and finally putforward a process of improving the removal of antibiotics in the existing wastewater treatment plants. Themain contents are as follows:
（1）Analyzed the pollution characteristics of SD and SMX in two sewage treatment plants of Tai'anCity by solid-phase extraction and high performance liquid chromatography (HPLC). The results showedthat influent concentration varies from different sources of sewage: The influent concentration of SD andSMX were165.8ng L-1and324.3ng L-1in Plant A for domestic sewage and the influent concentrationswere88.9and165.3ng L-1in Plant B for industrial wastewater; that removal rates varied from differentprocesses: the removal rates of SD and SMX in Plant A and B were48.3%、44.9%and39.1%、35.8%respectively; that the removal rates varied from different sections in Plant A, and the highest removalefficiency took place in aerobic cells, in which removal rates of SD and SMX were29.0%and20.6%%;that the removal mechanisms of SD and SMX were mainly adsorbed into particulate matter and theconcentrations of SD and SMX in concentrated sludge were135.4and285.3ng g-1.
（2） Optimized the parameters of removing two sulfa antibiotics in the SBR wastewater process byextending the sludge reaction time (SRT) and hydraulic reaction time (HRT). Experimental results showedthat extending the total HRT, improving the proportion of aerobic period-anaerobic period and extending the SRT contributed to the removal rates of SD and SMX: when the total HRT was480min, the SRT was25d, and the aerobic to anaerobic ratio was0.83, the removal rates of SD and SMX maintained at48~56%,51~58%;
(3) Strengthened the efficiency of the removal of two antibiotics in the sewage system by usingFenton reagent method, ferrate method and adsorption method. Experimental results showed that when thedischarge of sewage was0.4L and the concentration of SD and SMX was1.0mg·L-1, for the method offerrate, the optimum dosage was0.15mmoL L-1, pH was from6to7, the temperature was25℃, and thebest reaction time was10min, when the removal rates of SD and SMX reached88.6%and88.9%; for theFenton reagent method，the removal rate increased with the oxidant and catalyst dosage increased, theoptimum dosage was Fe2+=0.015mmoL L-1, H12O2=0.2mmoL L-, the initial reaction pH was4, thetemperature was25℃, the best reaction time was60min, the removal rates of SD and SMX reached92%and over99%; for the microporous resin adsorption method, the optimal dosage was1.6g, pH was from6to7, the equilibrium time was120min, absorption temperature was20℃, the removal rates of SD andSMX were80.8%and88.2%，and the removals of SD and SMX’s were in line with the first order kineticsmodel; when using activated carbon to remove SD and SMX, the optimum dosage was100mg, pH wasfrom6to7, the equilibrium time was180min., the removal rates of SD and SMX reached79.7%and91.5%and the removals of SD and SMX’s were in line with the first order kinetics model.
Meanwhile，the experimental results showed that optimized SBR technology could maintain theoriginal removal efficiency for the conventional indicators such as COD; that the advanced treatment is notso effective for the conventional indicators, and the removal rate was only about10%~35%; in sewagesystems of conventional biological treatment，increasing the depth treatment could effectively removeconventional pollutants and trace contaminants in sewage.
引文
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