Occurrence and fate of typical antibiotics in wastewater treatment plants in Harbin,North-east China

• The concentration distributions and removals of 12 antibiotics were investigated. • Macrolides and fluoroquinolones presented relatively higher concentrations. • The removal of antibiotics did not differ among the different treatment processes. As a new pollutant, antibiotics in the environment and their removal in wastewater treatment plants (WWTPs) have gained considerable attention. However, few studies investigated antibiotics in the north-eastern areas of China. By employing high-performance liquid chromatography-tandem mass spectrometry, the concentration distribution and removal of 12 antibiotics belonging to four types (cephalosporins, sulfonamides, fluoroquinolones, and macrolides) were investigated in influents and effluents as well as the removal efficiencies of four typical treatment processes in 18 wastewater treatment plants of Harbin City, north-eastern China. Macrolides and fluoroquinolones presented relatively higher detection concentrations and rates both in the water and in the sludge phases. Sulfonamides and cephalosporins displayed higher detection concentrations in the water phase. The representative antibiotics in influents and effluents included ROX, NOR, OFL, SMX, AZI, and CLA, with detection rates above 95%. The detection rates of the other six antibiotics exceeded 30%. In the sludge, the other five antibiotics, except SMX, presented relatively higher detection concentrations and rates, with detection rates greater than 95%. For cephalosporin, the detection rates of CTX and CFM in the sludge were 0. The removal efficiencies for the 12 antibiotics differed greatly, with average values ranging from 30% to 80% and the highest values for cephalosporin. The removal of antibiotics did not differ significantly among the four different treatment processes.     

Fenton试剂-硫酸镁深度处理酵母废水实验研究

采用Fenton试剂-硫酸镁对广东某酵母厂经厌氧、好氧、缺氧处理后的酵母废水进行深度处理。实验结果表明:采用Fenton试剂,在初始pH值为9、H2O2用量为5.55g/L、Fe2 加入量为1.41g/L、反应时间为20min的条件下,废水COD去除率达90%;继续采用硫酸镁对上清液进行处理,在调节pH为11～11.5、加入硫酸镁0.25～1.0g/L时,出水COD可降至138.0mg/L,颜色清澈。出水水质可达到《污水综合排放标准》(GB8978—1996)的二级标准。     

Occurrence,removal, and environmental risks of pharmaceuticals in wastewater treatment plants in south China

Pharmaceutically active compounds in wastewater released from human consumption have received considerable attention because of their possible risks for aquatic environments. In this study, the occurrence and removal of 10 pharmaceuticals in three municipal wastewater treatment plants in southern China were investigated and the environmental risks they posed were assessed. Nifedipine, atenolol, metoprolol, valsartan and pravastatin were detected in the influent wastewater. The highest average concentration in the influents was observed for metoprolol (164.6 ng/L), followed by valsartan (120.3 ng/L) in August, while median concentrations were higher in November than in August. The total average daily mass loadings of the pharmaceuticals in the three plants were 289.52 mg/d/person, 430.46 mg/d/person and 368.67 mg/d/person, respectively. Elimination in the treatment plants studied was incomplete, with metoprolol levels increasing during biological treatment. Biological treatment was the most effective step for PhACs removal in all of the plants studied. Moreover, the removal of PhACs was observed with higher efficiencies in August than in November. The WWTP equipped with an Unitank process exhibited similar removals of most PhACs as other WWTPs equipped with an anoxic/oxic (A/O) process or various anaerobic-anoxic-oxic (A²/O) process. The environmental risk assessment concluded that all of the single PhAC in the effluents displayed a low risk (RQ<0.1) to the aquatic environments.

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北江流域抗生素污染水平和来源初探

北江是发源于湖南(武水)和江西(浈水),汇于广东韶关,流经广东全境并入海的三大河流之一。为了解整个北江抗生素污染情况,共设置44个采样点,并采集了河水及部分沉积物样品,较全面地分析了各样品中12种典型抗生素含量并初步探究了其污染来源。研究发现,包括北江源头在内的全河段均有抗生素的检出,5类抗生素在表层水和沉积物中的平均浓度分别为77.8 ng·L~(-1)和3.6 ng·g~(-1)。其中,大环内酯类污染最为严重,其含量范围为11.7~114.6 ng·L~(-1)和0~435.3 ng·g~(-1),远高于其他类抗生素。表层水中磺胺类的磺胺甲恶唑和氯霉素类的检出率达100%,其中以磺胺甲恶唑(14.7 ng·L~(-1))和阿奇霉素(25.0 ng·L~(-1))为主,而沉积物中以阿奇霉素(35.9 ng·g~(-1))、氧氟沙星(5.4 ng·g~(-1))和四环素(3.3 ng·g~(-1))为主。由于流域污染源种类和数量不同,各抗生素在北江中的分布也存在差异。表层水中抗生素含量水平表现为下游高于上中游,在沉积物中则主要集中于中、下游之间河段。这反映了人类活动强度对北江抗生素污染的直接影响。     

以有机污染为主的河流治理技术研究进展

借鉴国外污染河流治理与修复的经验,并结合我国当前严重的河流污染形势,介绍了以有机污染为主的河流治理技术的研究进展。根据污染河水处理系统与河道的相对空间关系,河流治理技术可分为三类,第一类是将河水引出河道水系,引入附近的污水处理厂进行处理的异地处理法,其中截污工程是异地处理法的关键;第二类是在河道内建设处理系统,沿程进行河水净化的原位处理法,如河道内的曝气法、投菌法、生物膜法和化学法等;第三类是在河岸带上建设处理系统,将河水分流其中进行处理的旁路处理法,如建于河岸上的人工湿地处理系统、氧化塘以及多种形式的生物床或生物反应器等,旁路处理法起着人工强化河岸带的作用,是目前受污染河流治理中值得关注的一条新思路。受污染河流的具体处理方法及空间位置的选择,需要根据实际情况而定。     

Models predicting the fate of pollutants in rivers

The spill of 2,4,‐D in the Rhine river was used to show the evolution from simple to sophisticated models. The first simulation was done with an analytical solution of the dispersion‐advection equation without elimination. Elimination was introduced in a second simulation. The third simulation was carried out with a numerical model. This included elimination and variable dispersion. The lack of data limited the use of very detailed models.     

Occurrence and migration of microplastics and plasticizers in different wastewater and sludge treatment units in municipal wastewater treatment plant

● Reduce the quantifying MPs time by using Nile red staining. ● The removal rate of MPs and PAEs in wastewater and sludge were investigated. ● MPs and PAEs were firstly analyzed during thermal hydrolysis treatment. ● The removal of PAEs from wastewater and sludge was mainly biodegradation. Microplastics (MPs) and plasticizers, such as phthalate esters (PAEs), were frequently detected in municipal wastewater treatment plants (MWTP). Previous research mainly studied the removal of MPs and PAEs in wastewater. However, the occurrence of MPs and PAEs in the sludge was generally ignored. To comprehensively investigate the occurrence and the migration behaviors of MPs and PAEs in MWTP, a series of representative parameters including the number, size, color, shape of MPs, and the concentrations of PAEs in wastewater and sludge were systematically investigated. In this study, the concentrations of MPs in the influent and effluent were 15.46±0.37 and 0.30±0.14 particles/L. The MP removal efficiency of 98.1% was achieved and about 73.8% of MPs were accumulated in the sludge in the MWTP. The numbers of MPs in the sludge before and after digestion were 4.40±0.14 and 0.31±0.01 particles/g (dry sludge), respectively. Fourier Transform Infrared Spectroscopy (ATR FT-IR) analysis showed that the main types of MPs were polyethylene terephthalate (PET), polypropylene (PP), polyethylene (PE), and polystyrene (PS). Six PAEs, including phthalate (DMP), diethyl phthalate (DEP), diisobutyl phthalate (DIBP), ortho dibutyl phthalate (DBP), butyl benzyl phthalate (BBP), and bis(2-ethyl) hexyl phthalate (DEHP), were detected in the MWTP. The concentrations of total PAEs (ΣPAEs) in the influent and effluent were 76.66 and 6.28 µg/L, respectively. The concentrations of ΣPAEs in the sludge before and after digestion were 152.64 and 31.70 µg/g, respectively. In the process of thermal hydrolysis, the number and size of MPs decreased accompanied by the increase of the plasticizer concentration.     

南方典型水源地及水产养殖区抗生素的复合污染特征及生态风险

抗生素作为生长促进剂和疾病预防控制药物在水产养殖领域得到广泛应用,目前在许多环境水体中检测到不同类型的抗生素。环境中抗生素的残留问题也是目前环境研究的热点问题之一。本研究选择南方某市8个水源地和5个典型水产养殖区作为研究对象,采用固相萃取、高效液相色谱串联三重四级杆质谱联用仪方法,调查了32种常用抗生素在水体中的含量水平和空间分布特征,揭示了抗生素的来源,并对其生态风险进行了评价。水源地共检出12种抗生素,浓度范围为0.12～44.6 ng·L~(-1),以磺胺甲噁唑含量最高;水产养殖区检出14种抗生素,浓度范围为0.95～716 ng·L~(-1),以氯四环素检出浓度最高。整体上水产养殖区抗生素的浓度高于水源地。抗生素浓度与环境因子的冗余分析表明,水产养殖和生活污水排放是水体中抗生素的主要来源。对检出的13种抗生素进行生态风险评价,单一抗生素而言,环丙沙星、氧氟沙星、磺胺嘧啶、氯四环素和脱水红霉素的风险商值大于0.01而小于0.1,表现为低风险。总抗生素风险商值加和在大部分水源地大于0.01而小于0.1,表现为低风险;总抗生素风险商值加和在2个水产养殖区大于0.1,表现为中等风险,水产养殖区抗生素的长期生态风险应该引起关注。     

Occurrence and fate of PPCPs in typical drinking water treatment plants in China

Environmental Geochemistry and Health - In this study, the occurrence and removal of twenty-nine pharmaceuticals and personal care products (PPCPs) in two water treatment plants (WTPs) in China...     

Mitigating microbiological risks of potential pathogens carrying antibiotic resistance genes and virulence factors in receiving rivers: Benefits of wastewater treatment plant upgrade

● Abundance of MAGs carrying ARG-VF pairs unchanged in rivers after WWTP upgrade. ● Upgrade of WWTPs significantly reduced diversity of pathogenic genera in rivers. ● Upgrade of WWTPs reduced most VF (ARG) types carried by potential pathogens in rivers. ● Upgrade of WWTPs narrowed the pathogenic host ranges of ARGs and VFs in rivers. Wastewater treatment plants (WWTPs) with additional tertiary ultrafiltration membranes and ozonation treatment can improve water quality in receiving rivers. However, the impacts of WWTP upgrade (WWTP-UP) on pathogens carrying antibiotic resistance genes (ARGs) and virulence factors (VFs) in rivers remain poorly understood. In this study, ARGs, VFs, and their pathogenic hosts were investigated in three rivers impacted by large-scale WWTP-UP. A five-year sampling campaign covered the periods before and after WWTP-UP. Results showed that the abundance of total metagenome-assembled genomes (MAGs) containing both ARGs and VFs in receiving rivers did not decrease substantially after WWTP-UP, but the abundance of MAGs belonging to pathogenic genera that contain both ARGs and VFs (abbreviated as PAVs) declined markedly. Genome-resolved metagenomics further revealed that WWTP-UP not only reduced most types of VFs and ARGs in PAVs, but also effectively eliminated efflux pump and nutritional VFs carried by PAVs in receiving rivers. WWTP-UP narrowed the pathogenic host ranges of ARGs and VFs and mitigated the co-occurrence of ARGs and VFs in receiving rivers. These findings underline the importance of WWTP-UP for the alleviation of pathogens containing both ARGs and VFs in receiving rivers.     

滤层厚度对慢滤池深度处理污水的性能影响

将慢滤池用于污水二级出水的深度处理,并利用小试装置研究了滤层厚度对慢滤池性能的影响。选取浊度、COD和色度三个指标,在滤层不同深度处多次取样,分析各指标沿滤层厚度的变化。结果表明,采用粒径为0．4～0．6mm,滤层厚度为800mm的石英砂做滤床时,慢滤池对二级出水具有较好的净化效果：当进水浊度、COD和色度分别为1.3～6．9NTU、30．4～70．0mg·L^-1和20．6°～57．6°时,平均去除率分别达到86．5％、45．0％和46．3％。从试验结果可以看出,慢滤池类似一个微缩的污水二级处理系统,滤层表面的粘性滤膜起到类似初沉池的作用,可以对各指标实现较好的去除,58．6％的浊度、52．7％的COD和45．7％的色度是在滤层上部去除的;慢滤池中部起到类似曝气池的作用,下部起到类似二沉池的作用,对水质指标也能实现一定的去除。     

上海市受纳污水河流中多溴联苯醚的生态风险评价

以上海市某污水处理厂出水及其受纳河流为研究对象,测定了19种多溴联苯醚(PBDEs)同系物的浓度和分布特征,估算了污水处理厂PBDEs的年度排放负荷,并初步评价了受纳污水河流PBDEs的生态风险水平.结果表明,污水、河流水体及沉积物中PBDEs的总浓度分别为5050 pg.L-1、1310 pg.L-1和3.8 ng.g-1干重,其中BDE-209为主要成分.在排污口下游,PBDEs并没有随距离的增加而明显降低.该污水厂每年通过污水排放的五溴、八溴和十溴联苯醚分别为2.2、5.1和56.2 g.生态风险评价表明,目前该污水厂污水受纳河流中PBDEs导致的生态风险较低.     

北京市郊再生水灌区土壤有机氯农药垂向分布特征

在北京市郊再生水灌区采用正三角型布点法进行了3个钻孔的采样工作,钻孔间隔为1m,从表层开始每隔0.5m取一个样,3个钻孔共36组样品,同时采集钻孔附近的灌溉水及地下水,分别测试了土壤的理化参数及其土壤、灌溉水及地下水中9种有机氯农药的质量分数。测试结果表明：表层土壤是有机氯农药的主要残留层,表层土壤中检出的DDTs和BHCs质量分数较高,分别为2814.21ng·kg^-1和1130.41ng·kg^-1,但均符合土壤环境质量一级标准,残留污染程度较轻;其他层位以七氯和艾氏剂为主要检出物,最高质量分数分别为1286.19ng·kg^-1和781.23ng·kg^-1;其中艾氏剂未在表层土壤中检出;灌区内未检出的γ-BHC和（DDE＋DDD）/DDT的计算值为1.80,都说明近期内没有新污染源的输入;检出的有机氯农药在土壤剖面上的迁移能力有HEP〉ALD〉BHCs〉DDTs〉HCB,与地下水中检出的规律一致。     

Preliminary survey of pharmaceutical residues in some important Romanian rivers

A number of important rivers of Romania were investigated for pharmaceutical and antifungal residues. In a post target approach analysis, a single-stage, high-resolution mass spectrometry was successfully applied for the screening of 43 pharmaceuticals and fungicides in water, using U-HPLC-Exactive Orbitrap MS at 50,000 full width at half maximum resolution. Detection was based on accurate masses and retention times. The study confirmed the presence of pharmaceuticals and antifungals such as diclofenac, sulfamethoxazole, carbamazepine, trimethoprim, thiabendazole, and clotrimazole, in water. Diclofenac and carbamazepine were the most frequently detected (eight samples); concentrations ranged from 5 to 50 ng L^?1. Low concentrations of griseofulvin were detected in the Prut River. Further monitoring studies should be carried out in order to fill the gaps of knowledge concerning the presence of pharmaceutical residues in Romanian water environment and to improve public understanding regarding the environmental risk of pharmaceutical contamination.     

典型抗生素类药物在珠江三角洲水体中的污染特征

采用固相萃取、液相色谱/串联质谱法调查了9种典型抗生素类药物在珠江三角洲重要水体(珠江、维多利亚港、深圳河与深圳湾)中的污染特征。结果显示,珠江广州河段(枯季)和深圳河抗生素药物污染严重,最高含量达1340ng·L-1,河水中大部分抗生素含量明显高于美国、欧洲等发达国家河流中药物含量,红霉素(脱水)、磺胺甲噁唑等与国外污水中含量水平相当甚至更高。受深圳河污染的影响,深圳湾不同区域水体在一定程度上也受到抗生素药物污染,含量在10～100ng·L-1水平。维多利亚港水体中,只有较低含量的喹诺酮和大环内酯类抗生素有检出。深圳湾和维多利亚港周边水产养殖废水的排放成为水体中抗生素污染的重要来源之一。     

高碑店湖表层水中雌激素的分布及其光降解影响因素

雌激素等内分泌干扰物在水体中普遍存在,其在再生水中的存在以及在水体中的迁移转化会产生潜在的健康和生态风险。光降解是水体中雌激素消除的主要途径之一,水体中共存的无机离子及有机质等对雌激素的光解存在不同的影响。对高碑店湖再生水体中雌激素的污染状况进行了调查,结果显示表层水中天然雌激素雌酮(E1)和人工合成雌激素17α-乙炔基雌二醇(EE2)的浓度最高。在模拟太阳光照射条件下对E1在水溶液中的降解规律及影响因素进行了研究,发现在模拟1 SUN的光密度条件下,15 min时E1降解率可达85%(C0=5μg·L-1),而氨氮对E1的光降解存在一定的抑制作用,并且抑制作用随着氨氮的升高而变大。与纯水系统相比,高碑店湖表层水基质中E1的光降解速率较低,说明整体上氨氮、HCO-3、浊度等因素对E1光降解产生的抑制作用占主导。对雌酮及其降解产物进行了红外光谱分析,结果显示1 720 cm-1对应的C=O键特征峰在光照时间为0、10和20 min样品中的强度逐渐减弱,而2 854 cm-1和2 925 cm-1对应的脂肪碳的C-H键特征峰先增强后减弱,可能是因为E1结构中的C-C=O发生了反应生成了C=C-OH,而随着反应的继续,C=C也被进一步氧化,但降解产物的结构需要进一步研究推断。随着E1的光降解,E1水溶液的内分泌干扰活性逐渐下降,氨氮虽然对E1的光降解有一定的抑制作用,但随着降解反应的进行E1水溶液的内分泌干扰活性依然呈下降趋势。     

Occurrence and removal of N-nitrosodimethylamine and its precursors in wastewater treatment plants in and around Shanghai

Six wastewater treatment plants （WWTPs） were investigated to evaluate the occurrence and removal of N-nitrosodimethylamine （NDMA）, NDMA formation potential （FP） and four specific NDMA precursors, dimethylamine （DMA）, trimethylamine （TMA）, dimethyl- formamide （DMFA） and dimethylaminobenzene （DMAB）. DMA and tertiary amines with DMA functional group commonly existed in municipal wastewater. Chemically enhanced primary process （CEPP） had no effect on removal of either NDMA or NDMA FP. In WWTPs with secondary treatment processes, considerable variability was observed in the removal of NDMA （19%-85%） and NDMA FP （16%-76%）, moreover, there was no definite relationship between the removal of NDMA and NDMA FP. DMA was well removed in all the six surveyed WWTPs; its removal efficiency was greater than 97%. For the removal of tertiary amines, biologic treatment processes with nitrification and denitrification had better removal efficiency than conventional activated sludge process. The best removal efficiencies for TMA, DMFA and DMAB were 95%, 68% and 72%, respectively. CEPP could remove 73% of TMA, 23% of DMFA and 36% of DMAB. After UV disinfection, only 17% of NDMA was removed due to low dosage of UV was applied in WWTP. Although chlorination could reduce NDMA precursors, NDMA concentration was actually increased after chlorination.     

Removal of pharmaceutical and personal care products by sequential ultraviolet and ozonation process in a full-scale wastewater treatment plant

The application of appropriate advanced treat- ment process in the municipal wastewater treatment plants （WWTPs） has become an important issue considering the elimination of emerging contaminants, such as pharma- ceutical and personal care products （PPCPs）. In the present study, the removal of 13 PPCPs belonging to different therapeutic classes by the sequential ultraviolet （UV） and ozonation process in a full-scale WWTP in Beijing was investigated over the course of ten months. Most of the target PPCPs were effectively removed, and the median removal efficiencies of individual PPCPs, ranging from -13% to 89%, were dependent on their reaction rate constants with molecular ozone. Noticeable fluctuation in the removal efficiencies of the same PPCPs was observed in different sampling campaigns. Nevertheless, the sequential UV and ozonation process still made a significant contribution to the total elimination of most PPCPs in the full-scale WWTP, by compensating for the poor or fluctuant removal performance of PPCPs by biologic treatment process.     

再生水灌溉对冬小麦生长和产量的影响

随着我国污水处理技术的发展,再生水生产能力得到了明显地提高,实现再生水农业安全利用,将开辟农业用水新途径。以冬小麦（Triticum aestivum）为对象,通过盆栽试验,研究了不同程度处理的再生水（二级再生水、三级再生水）对冬小麦生长和产量的影响。结果表明：再生水灌溉能显著提高冬小麦的株高、叶面积、叶绿素含量,但开花前对光合作用的改善不显著。再生水灌溉处理的冬小麦超氧化物歧化酶（SOD）活性整体提高,尤其是越冬阶段,叶片SOD活性较对照处理提高了15%,抽穗后作用减弱,各处理间的过氧化物酶（POD）活性差异不明显。以再生水灌溉的盆栽小麦产量和对照相比没有明显差异,再生水灌溉可以实现正常的产量水平。     

光电催化转盘电极处理罗丹明B(RhB)模拟废水模型

在转盘式光电液膜反应器(RPEC)反应动力学方程的基础上,综合考虑外加偏压(0—0.4 V)、转盘转速(0—90 r.min-1)、初始浓度(0—100 mg.L-1)、转盘半径(37.5 mm)等因素对反应过程的影响,运用MATLAB软件对转盘转动的反应过程进行模拟计算和推测.计算结果与实验数据能较好吻合,数据误差在10%以内.从而建立了一种不同条件下转盘式光电催化降解废水的降解模型,对实际工业应用具有一定的预测与指导意义.