Removal of estrogens in municipal wastewater treatment under aerobic and anaerobic conditions: consequences for plant optimization

The removal of estrogens (estrone E1, estradiol E2, and ethinylestradiol EE2) was studied in various municipal wastewater treatment processes equipped for nutrient removal. A biological degradation model is formulated, and kinetic parameters are evaluated with batch experiments under various redox conditions. The resulting model calculations are then compared with sampling campaigns performed on differenttypes of full-scale plant: conventional activated-sludge treatment, a membrane bioreactor, and a fixed-bed reactor. The results show a > 90% removal of all estrogens in the activated sludge processes. (Due to the analytical quantification limit and low influent concentrations, however, this removal efficiency represents only an observable minimum.) The removal efficiencies of 77% and > or = 90% for E1 and E2, respectively, in the fixed-bed reactor represent a good performance in view of the short hydraulic retention time of 35 min. The first-order removal-rate constant in batch experiments observed for E2 varied from 150 to 950 d(-1) for a 1 gSS L(-1) sludge suspension. The removal efficiency of E1 and EE2 clearly depends on the redox conditions, the maximum removal rate occurring under aerobic conditions when E1 was reduced to E2. Sampling campaigns on full-scale plants indicate that the kinetic values identified in batch experiments (without substrate addition) for the natural estrogens may overestimate the actual removal rates. Although this paper does not give direct experimental evidence, it seems that the substrate present in the raw influent competitively inhibits the degradation of E1 and E2. These compounds are therefore removed mainly in activated sludge compartments with low substrate loading. Theoretical evaluation leads us to expect that diffusive mass transfer inside the floc (but not across the laminar boundary layer) appreciably influences the observed degradation rates of E1 and E2, but not of EE2.     

Fate of steroid estrogens in Australian inland and coastal wastewater treatment plants

A comparison of estrone (E1), 17beta-estradiol (E2), and 17alpha-ethinylestradiol (EE2) removal at a coastal enhanced primary and inland advanced sewage treatment plant (STP) is reported. The average concentration of estrogens in the raw sewage is similar to that reported in other studies. The sequential batch reactor at the advanced STP removed on average 85% of the incoming E1 and 96% of the E2. Further removal was observed during later microfiltration with the estrogen concentration below detection (<0.1 ng x L(-1)) after reverse osmosis. Some 6% of the influent E1+E2 was removed in the waste activated sludge. The detection of EE2 in the waste activated sludge (0.42 ng x g(-1) solids dry weight), undetectable in the raw sewage, suggests that EE2 is resistant to biological treatment in the sequential batch reactor and is primarily removed due to sorption. Little estrogen removal was observed at the enhanced primary with only 7% of E1 and 0% of E2 removed. Low removal is expected based on the degree of estrogens partitioning in the organic fraction given the relatively low solids concentration, but surprisingly, some 43% of E2, 24% of E1, and 100% of EE2 remains associated with the solids fraction in the treated effluent. Further research is necessary to determine whether the low level of estrogen removal for the coastal treatment plant will adversely affect the receiving marine environment.     

Removal of antibiotics in wastewater: Effect of hydraulic and solid retention times on the fate of tetracycline in the activated sludge process

A study was conducted to examine the influence of hydraulic retention time (HRT) and solid retention time (SRT) on the removal of tetracycline in the activated sludge processes. Two lab-scale sequencing batch reactors (SBRs) were operated to simulate the activated sludge process. One SBR was spiked with 250 microg/L tetracycline, while the other SBR was evaluated at tetracycline concentrations found in the influent of the wastewater treatment plant (WWTP) where the activated sludge was obtained. The concentrations of tetracyclines in the influent of the WWTP ranged from 0.1 to 0.6 microg/L. Three different operating conditions were applied during the study (phase 1-HRT: 24 h and SRT: 10 days; phase 2-HRT: 7.4 h and SRT: 10 days; and phase 3-HRT: 7.4 h and SRT: 3 days). The removal efficiency of tetracycline in phase 3 (78.4 +/- 7.1%) was significantly lower than that observed in phase 1 (86.4 +/- 8.7%) and phase 2 (85.1 +/- 5.4%) at the 95% confidence level. The reduction of SRT in phase 3 while maintaining a constant HRT decreased tetracycline removal efficiency. Sorption kinetics reached equilibrium within 24 h. Batch equilibrium experiments yielded an adsorption coefficient (Kads) of 8400 +/- 500 mL/g and a desorption coefficient (Kdes) of 22 600 +/- 2200 mL/g. No evidence of biodegradation for tetracycline was observed during the biodegradability test, and sorption was found to be the principal removal mechanism of tetracycline in activated sludge.     

Relationship between solid retention time and phosphorus removal in anaerobic-intermittent aeration process

Solid retention time (SRT) is one of the most important control parameters in biological phosphorus removal. In this study, lab-scale biological nutrient removal (BNR) reactors using anaerobic-intermittent aeration (AIA) were operated at various SRTs (i.e., 15, 20, and 30 d) to evaluate their phosphorus removal efficiencies. Sludge wasting load decreased as SRT increased; however, the phosphorus content in the biomass increased as SRT increased. The highest phosphorus removal efficiency was 93% at an SRT of 20 d and the phosphorus wasting load was also highest at that SRT, which indicates that the optimal SRT for the highest phosphorus removal is not proportional to the phosphorus content in the biomass. Aerobic digestion experiments were also carried out to determine the number of phosphate-accumulating organisms (PAOs) in the biomass produced in different reactors. All three activated sludges from BNR at SRTs of 15, 20, and 30 d showed a slower volatile suspended solid (VSS) destruction rate and a larger amount of phosphorus released than the conventional activated sludge (CAS), suggesting that the activated sludge from BNR has more PAOs than CAS. Also, the sludge at an SRT of 30 d showed a slower VSS destruction rate and a larger amount of phosphorus released than the sludge at an SRT of 15 d, suggesting that PAOs are more predominant at longer SRTs. Thus, to improve phosphorus removal efficiency, it is recommended that SRT be increased to maximize the number of PAOs in the system and that SRT be determined to maximize phosphorus wasting load.     

Fate of surfactants in membrane bioreactors and conventional activated sludge plants

Two membrane bioreactors (MBRs) were operated at high sludge retention time (SRT) (between 30 and 75 d) in parallel to a conventional activated sludge plant (CASP) conducted at SRT = 10 d. The fate of linear alkylbenzene sulfonate (LAS), nonylphenol ethoxylates (NP(n)EO, n = 1-15), nonylphenoxy carboxylates (NP(n)EC, n = 1-2), and nonylphenol (NP) in these systems was investigated. All systems were very efficient in the removal of LAS (around 99%). The analysis of variance showed that the difference in the removal efficiency of LAS in the CASP and the MBR operated at SRT = 65-75 d (respectively 99.0 ± 0.43 and 99.8 ± 0.11) were significant (p < 0.05), confirming the importance of SRT in the removal of LAS. Comparison between the CASP and the MBRs in the removal efficiency of nonylphenolic compounds were conducted considering NP(3-15)EO, the sum of NP(1-15)EO, NP(1-2)EC, and nonylphenol (NP). In all cases MBRs were more efficient than the CASP. In the case of NP the removal was about 76 ± 7.5% for the CASP and 90% ± 12.1 and 82 ± 8.7% for the MBRs. Better performance of MBRs in the removal of nonylphenolic compounds can be attributed to a better degradation. For example, if the sum of NP(1-15)EO and NP(1-2)EC is considered, estimated biodegradation was about 48% for the CASP and 72% for MBRs.     

Segregation of biomass in cyclic anaerobic/aerobic granular sludge allows the enrichment of anaerobic ammonium oxidizing bacteria at low temperatures

A cyclic anaerobic/aerobic bubble column reactor was run for 420 days to study the competition for nitrite between nitrite oxidizing bacteria (NOB) and anaerobic ammonium oxidizing bacteria (Anammox) at low temperatures. An anaerobic feeding period with nitrite and ammonium in the influent followed by an aerated period was applied resulting in a biomass specific conversion rate of 0.18 ± 0.02 [gN(2) - N · gVSS(-1)· day(-1)] when the dissolved oxygen concentration was maintained at 1.0 mgO(2) · L(-1). An increase in white granules was observed in the reactor which were mainly located at the top of the settled sludge bed, whereas red granules were located at the bottom. FISH, activity tests, and qPCR techniques revealed that red biomass was dominated by Anammox bacteria and white granules by NOB. Granules from the top of the sludge bed were smaller and therefore had a higher aerobic volume fraction, a lower density, and consequently a slower settling rate. Sludge was manually removed from the top of the settled sludge bed to selectively remove NOB which resulted in an increased overall biomass specific N-conversion rate of 0.32 ± 0.02 [gN(2) - N · gVSS(-1) · day(-1)]. Biomass segregation in granular sludge reactors gives an extra opportunity to select for specific microbial groups by applying a different SRT for different microbial groups.     

SBR法对缫丝废水的后续处理试验研究

通过研究影响序批式活性污泥法(SBR法)对缫丝废水的后续处理效果的各种因素,得出最佳工况运行条件。结果表明,在SBR法中,曝气时间为8 h,沉淀时间为40 min,溶解氧值为2～3 mg/L时,系统处理效果最好,COD、氨氮和TP的去除率分别达到90.5%±0.5%、95.1%±0.6%和78.2%±3.1%,出水的COD和氨氮都能达标排放。将SBR反应器作为缫丝废水后续好氧处理工艺,具有较高的处理效率和较好的运行稳定性。     

Enhanced biodegradation of iopromide and trimethoprim in nitrifying activated sludge

Iopromide (an X-ray contrast agent) and trimethoprim (an antibacterial drug) are frequently detected pharmaceuticals in effluents of wastewater treatment plants (WWTPs) and in surface waters due to their persistence and high usage. Laboratory-scale experiments showed that a significantly higher removal rate in nitrifying activated sludge as compared to conventional activated sludge was observed for both iopromide and trimethoprim. When the activity of the nitrifying bacteria was inhibited, the percent removal of iopromide decreased from 97 to 86% while trimethoprim removal decreased from 70 to 25%. The metabolite of iopromide identified when nitrification was not inhibited was a dehydroxylated iopromide at the two side chains. However, when the nitrifying bacteria were inhibited the metabolite identified was a carboxylate, formed during the oxidation of the primary alcohol on the side chain of iopromide. These results suggest that the nitrifying bacteria are important in the observed biodegradation of iopromide in the activated sludge with higher solid retention time (SRT). Results from the laboratory-scale study were corroborated by the observed removal efficiencies in a full-scale municipal WWTP, which showed that iopromide (ranging from 0.10 to 0.27 microg/L) and trimethoprim (ranging from 0.0.08 to 0.53 microg/L) were removed more effectively in the nitrifying activate sludge which has a higher SRT (49 days) than in the conventional activated sludge (SRT of 6 days). In nitrifying activated sludge, the percent removal of iopromide in the WWTP reached 61%, while in conventional activated sludge, average removal was negligible. For trimethoprim, removal was limited to about 1% in the conventional activated sludge, while in the nitrifying activated sludge, the removal was increased to 50%.     

Start-up of autotrophic nitrogen removal reactors via sequential biocatalyst addition

A procedure for start-up of oxygen-limited autotrophic nitrification-denitrification (OLAND) in a lab-scale rotating biological contactor (RBC) is presented. In this one-step process, NH4+ is directly converted to N2 without the need for an organic carbon source. The approach is based on a sequential addition of two types of easily available biocatalyst to the reactor during start-up: aerobic nitrifying and anaerobic, granular methanogenic sludge. The first is added as a source of aerobic ammonia-oxidizing bacteria (AAOB), the second as a possible source of planctomycetes including anaerobic ammonia-oxidizing bacteria (AnAOB). The initial nitrifying biofilm serves as a matrix for anaerobic cell incorporation. By subsequently imposing oxygen limitation, one can create an optimal environment for autotrophic N removal. In this way, N removal of about 250 mg of N L(-1) d(-1) was achieved after 100 d treating a synthetic NH4+-rich wastewater. By gradually imposing higher loads on the reactor, the N elimination could be increased to about 1.8 g of N L(-1) d(-1) at 250 d. The resulting microbial community was compared with that of the inocula using general bacterial and AAOB- and planctomycete-specific PCR primers. Subsequently, the RBC reactor was shown to treat a sludge digestor effluent under suboptimal and strongly varying conditions. The RBC biocatalyst was also submitted to complete absence of oxygen in a fixed-film bioreactor (FFBR) and proved able to remove NH4+ with NO2- as electron acceptor (maximal 434 mg of NH4+-N (g of VSS)(-1) d(-1) on day 136). DGGE and real-time PCR analysis demonstrated that the RBC biofilm was dominated by members of the genus Nitrosomonas and close relatives of Kuenenia stuttgartiensis, a known AnAOB. The latter was enriched during FFBR operation, but AAOB were still present and the ratio planctomycetes/AAOB rRNA gene copies was about 4.3 after 136 d of reactor operation. Whether this relates to an active role of AAOB in the anoxic N removal process remains to be solved.     

制革废水处理方法试验

探索折流式厌氧反应器法与序批式活性污泥法相结合的制革废水处理工艺,以折流式厌氧反应器法（ABR）水解制革废水中的难降解物质,去除大部分有机物后,再以序批式活性污泥法（SBR）通过硝化与反硝化反应,有效去除废水中的氨氮,从而使氨氮含量达标,与传统工艺相比,其效果明显,可使制革废水达到二级污水排放标准。     

Enhanced treatment efficiency of an anaerobic sequencing batch reactor (ASBR) for cassava stillage with high solids content

Cassava stillage is a high strength organic wastewater with high suspended solids (SS) content. The efficiency of cassava stillage treatment using an anaerobic sequencing batch reactor (ASBR) was significantly enhanced by discharging settled sludge to maintain a lower sludge concentration (about 30 g/L) in the reactor. Three hydraulic retention times (HRTs), namely 10 d, 7.5 d, 5 d, were evaluated at this condition. The study demonstrated that at an HRT of 5 d and an organic loading rate (OLR) of 11.3 kg COD/(m³ d), the total chemical oxygen demand (TCOD) and soluble COD (SCOD) removal efficiency can still be maintained at above 80%. The settleability of digested cassava stillage was improved significantly, and thus only a small amount of settled sludge needed to be discharged to maintain the sludge concentration in the reactor. Furthermore, the performance of ASBR operated at low and high sludge concentration (about 79.5 g/L without sludge discharged) was evaluated at an HRT of 5 d. The TCOD removal efficiency and SS in the effluent were 61% and 21.9 g/L respectively at high sludge concentration, while the values were 85.1% and 2.4 g/L at low sludge concentration. Therefore, low sludge concentration is recommended for ASBR treating cassava stillage at an HRT 5 d due to lower TCOD and SS in the effluent, which could facilitate post-treatment.     

Start-up, microbial community analysis and formation of aerobic granules in a tert-butyl alcohol degrading sequencing batch reactor

We demonstrate that compact well-settling aerobic granules can be developed in a sequencing batch reactor (SBR) for the biological removal of tert-butyl alcohol (TBA) using a strategy involving step increases in TBA loading rate achieved through increasing TBA concentrations in the influent. A moderate selection pressure that included a cycle time of 24 h and a start-of-cycle TBA concentration of 100 mg/L was initially introduced to encourage the growth and retention of biomass and avoid biomass loss from hydraulic washout. Start-of-cycle TBA concentrations were increased to 150, 300, 450, and 600 mg/L on days 90, 100, 121, and 199, respectively. These increases were only introduced after complete TBA removal was accompanied by visible improvements in biomass concentration and biomass settling ability. This acclimation strategy produced incrementally higher biomass concentrations and better settling biomass with higher specific TBA biodegradation rates. Effluent TBA concentrations were consistently below the detection limit of 25 microg/L. Aerobic granules were first observed about 180 days after reactor start-up. The granules had a clearly defined shape and appearance, settled significantly faster than the suspended sludge in the reactor, and eventually became the dominant form of biomass in the reactor. The adapted granules were capable of complete TBA removal and contained a stable microbial population with a low diversity of sequences of community 16S rRNA gene fragments. This study indicates that it is possible to use aerobic granules for TBA remediation and will contribute to a better understanding of how microbial acclimation can be exploited in the SBR to biologically remove recalcitrant xenobiotics.     

A comparison of two bench‐scale anaerobic systems used for the treatment of dairy effluents

The objective of this work was to compare two anaerobic reactor configurations, a hybrid upflow anaerobic sludge blanket (UASBh) reactor and an anaerobic sequencing batch reactor with immobilised biomass (ASBBR) treating dairy effluents. The reactors were fed with effluent from the milk pasteurisation process (effluent 1—E1) and later with effluent from the same process combined with the one from the cheese manufacturing (effluent 2—E2). The ASBBR reactor showed average organic matter removal efficiency of 95.2% for E1 and 93.5% for E2, while the hybrid UASB reactor showed removal efficiencies of 90.3% and 80.1% respectively.     

Biodegradation of p-nitrophenol by aerobic granules in a sequencing batch reactor

In this study, aerobic granules to treat wastewater containing p-nitrophenol (PNP) were successfully developed in a sequencing batch reactor (SBR) using activated sludge as inoculum. A key step was the conditioning of the activated sludge seed to enrich for biomass with improved settleability and higher PNP degradation activity by implementing progressive decreases in settling time and stepwise increases in PNP concentration. The aerobic granules were cultivated at a PNP loading rate of 0.6 kg/ m3 x day, with glucose to boost the growth of PNP-degrading biomass. The granules had a clearly defined shape and appearance, settled significantly faster than activated sludge, and were capable of nearly complete PNP removal. The granules had specific PNP degradation rates that increased with PNP concentration from 0 to 40.1 mg of PNP/L, peaked at 19.3 mg of PNP/(g of VSS) x h (VSS = volatile suspended solids), and declined with further increases in PNP concentration as substrate inhibition effects became significant. Batch incubation experiments show that the PNP-degrading granules could also degrade other phenolic compounds, such as hydroquinone, p-nitrocatechol, phenol, 2,4-dichlorophenol, and 2,6-dichlorophenol. The PNP-degrading granules contained diverse microbial morphotypes, and PNP-degrading bacteria accounted for 49% of the total culturable heterotrophic bacteria. Denaturing gradient gel electrophoresis analysis of 16S rRNA gene fragments showed a gradual temporal shift in microbial community succession as the granules developed from the activated sludge seed. Specific oxygen utilization rates at 100 mg/L PNP were found to increase with the evolution of smaller granules to large granules, suggesting that the granulation process can enhance metabolic efficiency toward biodegradation of PNP. The results in this study demonstrate that it is possible to use aerobic granules for PNP biodegradation and broadens the benefits of using the SBR to target treatment of toxic and recalcitrant organic compounds.     

The anaerobic conversion of methanol under thermophilic conditions: pH and bicarbonate dependence

The thermophilic (55 degrees C) anaerobic conversion of methanol was studied in an unbuffered medium (pH 4+/-0.2) and in a phosphate buffered medium (pH 6.4+/-0.1), in both cases without bicarbonate addition. Our cultivated sludge consortium was unable to degrade methanol under acidic conditions. During the 160 d of continuous operation of an up-flow anaerobic sludge blanket (UASB) reactor (R1), at an organic loading rate (ORL) of 6 gCOD/(l.d) and pH around 4, only 5% of the applied methanol load was consumed and no methane (CH4) was detected. However, hydrogenotrophic methanogens were found to be resistant to exposure to such conditions. At the end of the trial, the hydrogenotrophic methanogenic activity of the sludge was 1.23+/-0.16 gCOD/(gVSS.d) at neutral pH. With methanol as the test substrate, the addition of bicarbonate led to acetate accumulation. A second reactor (R2) was operated for 303 d at OLRs ranging from 5.5 to 25.4 gCOD/(l.d) in order to assess the conversion of methanol at neutral pH (phosphate buffered) in a bicarbonate deprived medium. The reactor performance was poor with a methanol-COD removal capacity limited to about 9.5 gCOD/(l.d). The system appeared to be quite susceptible to any type of disturbance, even at low OLR. The fraction of methanol-COD converted to CH4 and acetate was found to be unaffected by the OLR applied. At the end of the trial, the outcome of the competition was about 50% methanogenesis and 50% homoacetogenesis.     

SBR工艺处理白酒废水的研究

采用SBR法处理白酒废水,通过试验确定最佳运行工况：瞬时进水,在厌氧、好氧、缺氧条件下分别依次搅拌2．5h、8h、3h,再曝气30min,然后沉淀排泥排水,周期为14h。在此工况下该工艺在去除有机物的同时可达到良好的脱氮除磷功能,出水达到一级排放标准。     

17alpha-ethinylestradiol transformation via abiotic nitration in the presence of ammonia oxidizing bacteria

Impacts of trace concentrations of estrogens on aquatic ecosystems are a serious environmental concern, with their primary source being wastewater treatment facility effluents. Increased removal of 17alpha-ethinylestradiol (EE2) has been reported for activated sludge treatment with long enough solids retention time for nitrification. Previous work based on batch tests with Nitrosomonas europaea and nitrifying activated sludge at high EE2 concentrations (>300 000 ng/L) and high NH4-N concentrations (>200 mg/L) has led to the hypothesis that ammonia oxidizing bacteria cometabolically degrade EE2. This work investigated EE2 transformation with N. europaea and Nitrosospira multiformis at environmentally relevant EE2 concentrations and LC-MS-MS to observe transformation products. Degradation of EE2 was not observed in batch tests with no NH4-N addition or with 10 mg/L NH4-N fed daily. At increased NH4-N concentrations (200-500 mg/L) EE2 transformation was observed, but the only detected products were nitrated EE2. Abiotic assays with growth medium confirmed EE2 removal by nitration, which is enhanced at low pH and high NO2-N concentrations. These results suggest that EE2 removal at low concentrations found in municipal treatment activated sludge systems is not due to cometabolic degradation by ammonia oxidizing bacteria, or to abiotic nitration, but most likely due to heterotrophic bacteria.     

不同类型污泥接种源培养的好氧颗粒污泥脱氮性能比较

分别以活性污泥和厌氧颗粒污泥培养的好氧颗粒污泥为对象，对成熟污泥颗粒的脱氮性能进行了比较研究。结果表明，颗粒污泥驯化成熟之后，对氨氮的去除效果维持在95％左右，与其污泥接种源没有明显的相关关系；对一个降解周期内氮的形态分析表明，在颗粒污泥存在的反应器内发生了同步硝化反硝化。     

采用IC厌氧反应器处理制浆造纸工厂废水

立式IC厌氧反应器与好氧结合处理废水,工艺水可封闭循环,实现废水零排放。采用IC厌氧反应器解决了活性污泥问题,消除泡沫和污泥疏松。年产量5万吨的纸板厂,废水处理车间COD去除率达85％～90％,在IC厌氧反应器中COD去除率为65％,并转化成生物气体（主要是甲烷）,得到的生物气体平均为1200-1500m^2／d。年产量30万t／年的纸板厂,废水处理车间COD和BOD除去率分别为72％和80％,在1C厌氧反应器中使有机污染物转化成生物气体,产生能量35000kWh／d。     

Treatment of liquid fraction separated from liquidized food waste in an upflow anaerobic sludge blanket reactor

Thermochemical liquidization as a pretreatment for anaerobic digestion of food waste was studied using a laboratory-scale upflow anaerobic sludge blanket (UASB) reactor for a period of 82 d. Model food waste (approximately 90 wt% moisture content) was thermochemically liquidized at 175 degrees C for 1 h. The liquidized food waste was separated into a solid phase (6-10 wt%) and a liquid phase (85-89 wt%). The diluted liquid phase was continuously treated by anaerobic digestion using a UASB reactor at 35 degrees C. The volumetric loading rate was increased stepwise to 6.4-7.2 g total organic carbon (TOC)/l-reactor/d. Methane production was found to be approximately 0.35-0.61 l/g-TOC removed. The range of TOC removal efficiencies was 67-69% at an influent TOC concentration of 10.1-11.1 g/l and a volumetric loading rate of 4.8-5.3 g-TOC/l-reactor/d. This treatment process using an UASB reactor could be suitable for resource recovery from food waste.