Biodegradation of triclosan and formation of methyl-triclosan in activated sludge under aerobic conditions

Triclosan is an antimicrobial agent which is widely used in household and personal care products. Widespread use of this compound has led to the elevated concentrations of triclosan in wastewater, wastewater treatment plants (WWTPs) and receiving waters. Removal of triclosan and formation of triclosan-methyl was investigated in activated sludge from a standard activated sludge WWTP equipped with enhanced biological phosphorus removal. The removal was found to occur mainly under aerobic conditions while under anoxic (nitrate reducing) and anaerobic conditions rather low removal rates were determined. In a laboratory-scale activated sludge reactor 75% of the triclosan was removed under aerobic conditions within 150 h, while no removal was observed under anaerobic or anoxic conditions. One percent of the triclosan was converted to triclosan-methyl under aerobic conditions, less under anoxic (nitrate reducing) and none under anaerobic conditions.     

A2O工艺中雌激素的行为变化和去除机理

研究了厌氧-缺氧-好氧(A2O)活性污泥工艺对生活污水中天然雌激素雌酮(Estrone,E1)、17β-雌二醇(17β-Estradiol,E2)以及17α-乙炔基雌二醇(17α-Ethynylestradiol,EE2)的去除性能。在对COD、N和P具有良好去除效果的前提下,对E1、E2和EE2的去除率可分别达到92.7%、100%和62.7%。通过对各反应单元内3种雌激素的物料平衡分析,表明A2O工艺对雌激素的去除主要发生在厌氧段和好氧段。以失活污泥作为对照组,好氧硝化过程中雌激素去除的小试实验发现,好氧过程中E1、E2的去除主要依靠生物降解作用,而EE2的去除则主要依赖于活性污泥对其的吸附作用。     

A^2O工艺中雌激素的行为变化和去除机理

研究了厌氧-缺氧-好氧（A2O）活性污泥工艺对生活污水中天然雌激素雌酮（Estrone,E1）、17β-雌二醇（17β-Estradiol,E2）以及17α-乙炔基雌二醇（17α-Ethynylestradiol,EE2）的去除性能。在对COD、N和P具有良好去除效果的前提下,对E1、E2和EE2的去除率可分别达到92.7%、100%和62.7%。通过对各反应单元内3种雌激素的物料平衡分析,表明A2O工艺对雌激素的去除主要发生在厌氧段和好氧段。以失活污泥作为对照组,好氧硝化过程中雌激素去除的小试实验发现,好氧过程中E1、E2的去除主要依靠生物降解作用,而EE2的去除则主要依赖于活性污泥对其的吸附作用。     

好氧硝化颗粒污泥膜生物反应器性能和膜污染研究

实验研究了好氧硝化颗粒污泥膜生物反应器AGMBR的处理性能,并将其与活性污泥膜生物反应器ASMBR进行对比,考察了颗粒污泥在减缓膜污染中所起的作用.好氧硝化颗粒污泥膜生物反应器AGMBR连续稳定运行102 d,系统具有良好的去除有机物和同时硝化反硝化能力,在进水COD和NH+4-N浓度分别为500和200 mg/L时,COD、NH+4-N和TN的去除率分别稳定在86%、94%和45%以上.颗粒污泥有效减缓了膜污染,延长了膜清洗的周期,AGMBR中的膜污染以膜孔堵塞为主,占总阻力的64.81%;滤饼层的阻力为2.1×1012m-1,远小于ASMBR中的16.07×10"m-1;膜清洗周期是相同条件下ASMBR的2.43倍以上;而且AGMBR内不断有新颗粒生成,维持了AGMBR系统性能和运行的稳定.     

好氧颗粒污泥处理高浓度氨氮废水的研究

在不同接种源污泥颗粒化过程中污泥理化性状对比研究的基础上,采用成熟好氧颗粒污泥处理高浓度氨氮废水,对其脱氮行为以及不同C/N条件下好氧颗粒污泥微生物的比耗氧速率、好氧颗粒污泥对氨氮的比降解速率随时间的变化等进行了研究.实验结果表明,在进水氨氮质量浓度较高(480 mg/L)、温度30℃左右的条件下,稳定运行15 d,氨氮的去除率维持在85%左右;进水氨氮的浓度越高,随着微生物对环境的逐渐适应,硝化菌的活性也逐步增加;随着进水氨氮浓度的提高,好氧颗粒污泥对氨氮的比降解速率也逐渐上升.     

Removal of selected natural and synthetic estrogenic compounds in a Canadian full-scale municipal wastewater treatment plant.

The effect of a full-scale municipal wastewater treatment plant (WWTP) and each of the treatment units within the stream on the removal of endocrine-disrupting compounds was evaluated by tracking 17-beta-estradiol (E2), estrone (E1), and 17-alpha-ethinylestradiol (EE2). The overall performance of the WWTP compared well with other plants, as 90.5% removal of E1+E2 and 74.9% removal of EE2 were observed. A larger fraction of EE2 entered the plant in particulate form than E1 and E2, while a lower fraction of EE2 left the plant in particulate form than soluble form. The activated sludge units reduced the concentration of E1+E2 and EE2 in the liquid phase by 88.2% and 44.6%, respectively. The UV treatment process did not reduce the amount of estrogens. The aqueous phase of the tertiary lagoon solids contained higher levels of estrogens compared with the lagoon influent.     

Degradation of ethinyl estradiol by nitrifying activated sludge

Degradation of ethinyl estradiol (EE2) by nitrifying activated sludge was studied with micro-organisms grown in a reactor with feedback of sludge fed with only a mineral salts medium containing ammonium as the sole energy source. Ammonium was oxidised by this sludge at a rate of 50 mg NH4+ g(-1) DW h(-1). This activated sludge was also capable of degrading EE2 at a maximum rate of 1 microg g(-1) DW h(-1). Using sludge with an insignificant nitrifying capacity of 1 mg NH4+ g(-1) DW h(-1), no degradation of EE2 was detected. Oxidation of EE2 by nitrifying sludge resulted in the formation of hydrophilic compounds, which were not further identified. Most probably degradation by nitrifying sludge results in a loss of estrogenic activity, as hydroxylated derivatives of EE2 are known to have a substantially lower pharmacological activity than EE2.     

Assessment of the importance of sorption for steroid estrogens removal during activated sludge treatment

Distribution coefficients (K(d)) between water and activated sludge particles (f(oc)=27.7+/-0.1%) were measured for the steroid estrogens (SE), estrone (E1), 17beta-estradiol (E2) and 17alpha-ethinylestradiol (EE2) in batch experiments. Experimental concentration levels ranged from environmentally realistic low ng/l to the high microg/l. In this range K(d)s were independent of their water concentration. The experimentally obtained K(d)s (with 95% confidence intervals) were 402+/-126 l/kg, 476+/-192 l/kg and 584+/-136 l/kg for E1, E2 and EE2, respectively. K(d)s were used to estimate the fraction of the total SE concentration that is expected to be sorbed in the activated sludge treatment tanks of a typical STP assuming equilibrium conditions. Assuming a suspended solids concentration of 4 g/l dissolved solids (ds), it was estimated that 61+/-9%, 66+/-13% and 70+/-6% of the total concentration of E1, E2 and EE2, respectively, would be sorbed during activated sludge treatment. The fraction of the SEs that was expected to be sorbed to suspended sludge particles in the effluents from a typical Danish STP was estimated to be only 0.20+/-0.06%, 0.24+/-0.10% and 0.29+/-0.07% of the total concentration of E1, E2 and EE2, respectively, at a suspended solids concentration of 5 mg/lds. For a typical STP the removal of steroid estrogens with excess sludge was estimated to be only 1.5-1.8% of the total loading if equilibrium conditions exists. Sorption is therefore not important for the fate of SEs in STPs compared to biodegradation.     

An analysis of nitrification during the aerobic digestion of secondary sludges

Investigations were undertaken to study the occurrence and progress of nitrification during aerobic digestion of activated sludge in a wide range of initial concentrations of total solids (1000 to 80 000 mg litre(-1), initial pH range of 4.5 to 10.4 and digestion temperature range of 5 degrees to 60 degrees C. Batch aerobic digestion studies on activated sludge grown on wastewater (enriched with organic solids from human excretal material) indicate that almost complete elimination of the 'biodegradable' matter of the activated sludge was one of the essential prerequisites to initiate nitrification. Favourable ranges of temperature and pH for nitrification were observed to be 25 degrees to 30 degrees C and 6.0 to 8.3, respectively. With all favourable conditions, a minimum period of about 2 days was necessary for population build-up of genera Nitrosomonas and Nitrobacter, and to initiate nitrification. Nitrate formation invariably lagged behind nitrite formation, but under certain conditions both phases of nitrification were observed to progress hand in hand.     

Xenobiotic benzotriazoles—biodegradation under meso- and oligotrophic conditions as well as denitrifying,sulfate-reducing,and anaerobic conditions

The intensive use of benzotriazoles as corrosion inhibitors for various applications and their application in dishwasher detergents result in an almost omnipresence of benzotriazole (BTri), 4-methyl- and 5-methyl-benzotriazole (4-TTri and 5-TTri, respectively) in aquatic systems. This study aims on the evaluation of the biodegradation potential of activated sludge communities (ASCs) toward the three benzotriazoles regarding aerobic, anoxic, and anaerobic conditions and different nutrients. ASCs were taken from three wastewater treatment plants with different technologies, namely, a membrane bioreactor (MBR-MH), a conventional activated sludge plant CAS-E (intermittent nitrification/denitrification), and CAS-M (two-stage activated sludge treatment) and used for inoculation of biodegradation setups. All ASCs eliminated up to 30 mg L^?1 5-TTri and BTri under aerobic conditions within 2–7 and 21–49 days, respectively, but not under anoxic or anaerobic conditions. 4-TTri was refractory at all conditions tested. Significant differences were observed for BTri biodegradation with non-acclimated ASCs from MBR-MH with 21 days, CAS-E with 41 days, and CAS-M with 49 days. Acclimated ASCs removed BTri within 7 days. Furthermore, different carbon and nitrogen concentrations revealed that nitrogen was implicitly required for biodegradation while carbon showed no such effect. The fastest biodegradation occurred for 5-TTri with no need for acclimatization, followed by BTri. BTri showed sludge-specific biodegradation patterns, but, after sludge acclimation, was removed with the same pattern, regardless of the sludge used. Under anaerobic conditions in the presence of different electron acceptors, none of the three compounds showed biological removal. Thus, presumably, aerobic biodegradation is the major removal mechanism in aquatic systems.     

Oxidation of natural and synthetic hormones by the horseradish peroxidase enzyme in wastewater

Steroid estrogens, including both natural estrogens (e.g., estrone - E1; 17beta-estradiol - E2; and estriol - E3) and synthetic estrogens (e.g., 17alpha-ethinylestradiol - EE2), are known as endocrine-disrupting compounds. The objective of this research was to evaluate the feasibility of the enzymatic oxidation of estrogens and to optimize this process in municipal wastewater contaminated with steroid estrogens using horseradish peroxidase (HRP) and hydrogen peroxide. An initial HRP activity of 0.02 U ml(-1) was sufficient to completely remove EE2 from the synthetic solution, although greater HRP doses (up to 0.06 U ml(-1)) were required to remove E1, E2 and E3. The optimal molar peroxide-to-substrate ratio was determined to be approximately 0.45. Based on the Michaelis-Menten kinetics, the HRP had an increasing reactivity with E1, E3, E2, and EE2, in increasing order. In real activated sludge process effluent, an HRP dose of 8-10 U ml(-1) was required to completely remove all of the studied estrogens, while only 0.032 U ml(-1) of HRP was necessary to treat synthetic water containing the same estrogen concentrations.     

Simultaneous nitrification and denitrification in an aerobic reactor with granular sludge originating from an upflow anaerobic sludge bed reactor.

Anaerobic granular sludge, obtained from an upflow anaerobic sludge bed reactor at a brewery waste treatment station, was cultured for 3 months under aeration conditions until the diameter of sludge was in the range 1.8 to 2.6 mm. The aerobic granular sludge gathered acquired the ability of catalyzing simultaneous nitrification and denitrification (SND) and was applied in the study of the process of nitrogen removal in a bioreactor. The ratio between chemical oxygen demand (COD) and ammonium-nitrogen (NH4(+)-N) concentration in the influent was found to be an important factor influencing the process of SND. The final percentage removal of NH4(+)-N reached 100% under the optimal condition of 500 mg/L COD and 0.39 NH4(+)-N/COD. Intermediate products, such as nitrite-nitrogen and nitrate-nitrogen, were also analyzed to clarify the SND process with the aerobic granular sludge.     

Fate of sex hormones in two pilot-scale municipal wastewater treatment plants: conventional treatment

The fate of seven sex hormones (estrone (E1), estradiol (E2), estriol (E3), ethinylestradiol (EE2), testosterone, androstenedione, and progesterone) was determined in two pilot-scale wastewater treatment plants operated under conventional loading conditions. The levels of hormones in both the liquid and the solid matrixes of the plants were determined. Each of the two 20-l/h pilot-scale plants consisted of a primary clarifier followed by a three-stage aeration tank and a final clarifier. The primary sludge and the waste activated sludge (WAS) were digested anaerobically in one pilot plant and aerobically in the other. The pilot plants were fed a complex synthetic wastewater spiked with the hormones. Levels of testosterone, androstenedione and progesterone were close to method detection limit (MDL) concentrations in the final and digester effluents (both liquid and solid phases) and were considered as completely removed. Average mass flux removals from the liquid streams (plant influent minus secondary clarifier effluent) for the natural estrogens were 82% for E1, 99% for E2, and 89% for (E1+E2). An average overall removal of only 42% was achieved for EE2. These values reflect removals averaged for the two pilot plants.     

Improving nitrogen removal in two modified decentralized wastewater systems

Efficient nutrient removal in decentralized wastewater treatment systems is a challenging task. To improve the removal of organic matter and nitrogen from wastewater, two types of bioreactors using membrane-aerated biofilm reactor (MABR) and microbial fuel cell (MFC) techniques were evaluated. During more than 250 days of continuous-flow reactor operation, both reactors showed consistently high chemical oxygen demand removal (>86%). At an influent ammonium-nitrogen (NH4(+)-N) concentration of 30 mg N/L, the average effluent NH4(+)-N concentrations were 6.2 and 0.5 mg N/L for the MABR and MFC reactor, respectively, while the effluent nitrate-nitrogen (NO3(-)-N) concentrations were 5.4 mg/ L in the MABR and 19.2 mg/L in the MFC-based reactor. The overall total inorganic nitrogen removal efficiencies were 64% and 36% for the MABR and MFC reactor, respectively. At the measured dissolved oxygen concentrations of 5.2 and 0.23 mg/L in the aerobic/anoxic zone of the MFC and MABR, respectively, a specific oxygen uptake rate of 0.1 g O2/g VSS-d, resulting from ammonia oxidation, was detected in the settled sludge of the MFC, while no nitrifying activity of the sludge from the MABR was detected. Molecular microbial analysis demonstrated a link between the bacterial community structure and nitrifying activity. The relatively high abundance of Nitrosomonas europaea was associated with its detectable nitrification activity in the settled sludge of the MFC. The results suggest that MABR and MFC techniques have the potential to improve organic and nitrogen removal in decentralized wastewater systems.     

硝化颗粒污泥的快速培养及其硝化特性分析

以好氧颗粒污泥接种小试柱形SBR,采用自配无机氨氮废水为进水,在中温（28～30℃）条件下通过逐步提升进水NH4^＋-N浓度（100～650mg／L）和缩短水力停留时间（8～4h）快速培养硝化颗粒污泥。实验结果证实,以好氧颗粒污泥接种可以促使硝化颗粒污泥快速形成,36d时粒径〉0．21mm的颗粒污泥占总数的93％,颗粒污泥NH4-N比去除速率为50．53mgNH4^＋-N／（gSS·h）。硝化颗粒污泥具有良好的短程硝化性能,亚硝酸盐产生速率和累积率分别保持在3．3kgNO2-N／（m^3·d）和85％以上。反应初期高FA和反应末期高FNA的共同抑制是该研究中实现和维持稳定短程硝化的关键因素。     

超声波促进城市生活污泥缺氧/好氧消化的研究

本研究将超声波预处理引入城市生活污泥缺氧/好氧消化工艺中,自主设计了容积为30 L的生活污泥超声波-缺氧/好氧消化中试系统并用以实验研究。超声波预处理的参数为超声频率28 kHz,声能密度0.15 W/mL,超声时间10 min,超声间隔12 h,污泥超声比例30%。结果表明,引入超声预处理后,缩短了污泥的稳定时间,提高了污泥的消化效率。污泥消化10 d就已经达到了稳定标准,比未引入超声预处理时缩短了12 d,而MLVSS最大去除率提高了11%,达到了55.10%。超声波的引入,对污泥缺氧/好氧消化系统中污泥上清液溶解性COD（SCOD）的变化趋势影响比较明显,而对上清液的pH、氨氮和TP的变化趋势没有明显影响。     

Microbial degradation of 17β -estradiol and 17α -ethinylestradiol followed by a validated HPLC-DAD method

This work aimed at studying the biodegradation of two estrogens, 17α -estradiol (E2) and 17β -ethinylestradiol (EE2), and their potential metabolism to estrone (E1) by microbial consortia. The biodegradation studies were followed by High Performance Liquid Chromatography–Diode Array Detector (HPLC–DAD) using a specifically developed and validated method. Biodegradation studies of the estrogens (E2 and EE2) were carried out with activated sludge (consortium A, CA) obtained from a Wastewater Treatment Plant (WWTP) and with a microbial consortium able to degrade recalcitrant compounds, namely fluorobenzene (consortium B, CB). E2 was more extensively degraded than EE2 by CA whereas CB was only able to degrade E2. The addition of acetate as a supplementary carbon source led to a faster biodegradation of E2 and EE2. E1 was detected as a metabolite only during the degradation of E2. The 16S rRNA gene sequence analyses of strains recovered from the degrading cultures revealed the presence of the genera Pseudomonas, Chryseobacterium and Alcaligenes. The genera Pseudomonas and Chryseobacterium were retrieved from cultures supplied with E2 and EE2, while the genus Alcaligenes was found in the presence of E2, suggesting that they might be involved in the degradation of these compounds.     

Simultaneous nitrification-denitrification and clarification in a pseudoliquified activated sludge system.

This paper describes results from a pilot study of a novel wastewater treatment technology, which incorporates nutrient removal and solids separation to a single step. The pseudoliquified activated sludge process pilot system was tested on grit removal effluent at flowrates of 29.4 to 54.7 m3/d, three different solid residence times (SRT) (15, 37, and 57 days), and over a temperature range of 12 to 28 degrees C. Despite wide fluctuations in the influent characteristics, the system performed reliably and consistently with respect to organics and total suspended solids (TSS) removals, achieving biochemical oxygen demand (BOD) and TSS reductions of > 96% and approximately 90%, respectively, with BOD5 and TSS concentrations as low as 3 mg/L. Although the system achieved average effluent ammonia concentrations of 2.7 to 3.2 mg/L, nitrification efficiency appeared to be hampered at low temperatures (< 15 degrees C). The system achieved tertiary effluent quality with denitrification efficiencies of 90 and 91% total nitrogen removal efficiency at a total hydraulic retention time of 4.8 hours and an SRT of 12 to 17 days. With ferric chloride addition, effluent phosphorous concentrations of 0.5 to 0.8 mg/L were achieved. Furthermore, because of operation at high biomass concentrations and relatively long biological SRTs, sludge yields were over 50% below typical values for activated sludge plants. The process was modeled using activated sludge model No. 2, as a two-stage system comprised an aerobic activated sludge system followed by an anoxic system. Model predictions for soluble BOD, ammonia, nitrates, and orthophosphates agreed well with experimental data.     

Comparison of nitrification rates in conventional and membrane-assisted biological nutrient removal processes

A membrane-assisted and a conventional activated sludge system, both operated in an enhanced biological phosphorus removal (EBPR) mode and under identical operating conditions, were studied to investigate the effect of the membrane solids-liquid separation on nitrification activity. Both the membrane EBPR (MEBPR) and conventional EBPR (CEBPR) processes achieved stable and complete removal of ammonium-nitrogen from the influent wastewater. However, when the intrinsic nitrification activity was assessed in offline batch tests, the CEBPR mixed liquor exhibited 15 to 75% greater nitrification potential than the MEBPR counterpart. These results were further validated by monitoring nitrification rates of conventional mixed liquor as it evolved toward a membrane mixed liquor. It was also demonstrated that the larger aerobic mass fraction of the MEBPR system could not be the only factor influencing the reduced intrinsic nitrification rate. The present study strongly suggests that the presence of a membrane solids-liquid separation per se may be sufficient to alter the nitrification kinetics of an EBPR mixed liquor and that this possibility should be considered in arriving at an appropriate process design.     

17 β-estradiol and 17 α-ethinylestradiol mineralization in sewage sludge and biosolids

Natural steroid estrogens (e.g., 17 β-estradiol, E2), synthetic steroid estrogens (e.g., 17 α-ethinylestradiol, EE2) and pharmaceutical antibiotics (e.g., ciprofloxacin) are chemicals detected in biosolids and sewage sludges because they partition into the solids fraction during the wastewater treatment process. This research utilized a three-way factorial design (six media × two estrogens × three antibiotic treatments) to quantify cumulative E2 and EE2 mineralization over 133 d (MAX) in a range of sewage sludge and biosolid samples in the presence (4 and 40 mg kg^?1) and absence of ciprofloxacin. The same three-way factorial design was utilized to quantify the impact of the six media, E2 or EE2, and ciprofloxacin on cumulative soil respiration over 133 d (RESP). Minimal ciprofloxacin mineralization was observed (<0.05% over 133 d), but despite its persistence, ciprofloxacin had no significant effect on MAX of E2 or EE2, and, in general, no significant effect on RESP. MAX ranged from 38.38% to 48.44% for E2 but from only 0.72% to 24.27% for EE2 although RESP was relatively similar, ranging from 101.00 to 866.54 mg CO₂ in the presence of E2 and from 69.55 to 893.95 mg CO₂ in the presence of EE2. The sorption-limited bioavailability of EE2, which is inherently resistant to biodegradation due to chemical structure, as MAX and Freundlich sorption coefficients (K_f) were negatively correlated. As such, the K_f values of EE2 were largest in composted biosolids in which EE2 was particularly resistant to microbial degradation as the MAX of EE2 was <3%. In contrast, the MAX of E2 showed a positive association with the K_f values of E2 because some steps in the E2 transformation process have been found to occur in the sorbed phase. The MAX of E2 was significantly greater in the biosolid and composted biosolid media than in any other media, whereas the MAX of E2 decreased in the following order: secondary sewage sludge > primary sewage sludge > biosolid = composted biosolid. This suggests that sewage sludges in municipal lagoons and pre-treatment holding lagoons are a more favorable media for mineralization of EE2, whereas biosolids in post-treatment storage lagoons are a more favorable media for the mineralization of E2. The presence of ciprofloxacin will have no impact on the potential E2 or EE2 mineralization rates in these cases.