Fate and removal of selected endocrine‐disrupting compounds in sewage using activated sludge treatment

The variation and fate of four endocrine‐disrupting compounds (EDCs) composed of 4‐n‐nonylphenol (4‐n‐NP), bisphenol A (BPA), 17β‐estradiol (E2) and 17α‐ethinylestradiol (EE2) were investigated along treatment units in a sewage treatment plant (STP), China with anaerobic, anoxic and aerobic activated sludge processes. The mean concentrations were 64.8 ng/L (E2), 115.3 ng/L (4‐n‐NP), 171.5 ng/L (EE2), and 920.7 ng/L (BPA) in the influents, and 22.8 ng/L (E2), 50.9 ng/L (4‐n‐NP), 49.9 ng/L (EE2), and 84.3 ng/L (BPA) in the effluents. The biological treatment was more effective in removing NP, BPA and E2 from the aqueous phase than the primary treatment, while the latter could effectively remove EE2. Their possible removal mechanisms during the biological treatment with activated sludge were further explored through spiked batch experiments under three oxygen‐supplying conditions (anaerobic, anoxic and aerobic). The batch experiments showed that 4‐n‐NP, E2 and BPA were removed from the aqueous phase through biodegradation. The combination of sludge sorption and biodegradation accounted for the removal of EE2. Anoxic activated sludge showed the most rapid degradation of 4‐n‐NP, while E2 could be removed most effectively by aerobic activated sludge, and sludge sorption had a remarkable effect on its removal within the initial 15 min of the experiments under three oxygen‐supplying conditions.     

The effect of thermal hydrolysis pretreatment on the anaerobic degradation of nonylphenol and short-chain nonylphenol ethoxylates in digested biosolids

The presence of micropollutants can be a concern for land application of biosolids. Of particular interest are nonylphenol diethoxylate (NP₂EO), nonylphenol monoethoxylate (NP₁EO), and nonylphenol (NP), collectively referred to as NPE, which accumulate in anaerobically digested biosolids and are subject to regulation based on the environmental risks associated with them. Because biosolids are a valuable nutrient resource, it is essential that we understand how various treatment processes impact the fate of NPE in biosolids. Thermal hydrolysis (TH) coupled with mesophilic anaerobic digestion (MAD) is an advanced digestion process that destroys pathogens in biosolids and increases methane yields and volatile solids destruction. We investigated the impact of thermal hydrolysis pretreatment on the subsequent biodegradation of NPE in digested biosolids. Biosolids were treated with TH, anaerobic digestion, and aerobic digestion in laboratory-scale reactors, and NPE were analyzed in the influent and effluent of the digesters. NP₂EO and NP₁EO have been observed to degrade to the more estrogenic NP under anaerobic conditions; therefore, changes in the ratio of NP:NPE were of interest. The increase in NP:NPE following MAD was 56%; the average increase of this ratio in four sets of TH-MAD samples, however, was only 24.6 ± 3.1%. In addition, TH experiments performed in pure water verified that, during TH, the high temperature and pressure alone did not directly destroy NPE; TH experiments with NP added to sludge also showed that NP was not destroyed by the high temperature and pressure of TH when in a more complex sludge matrix. The post-aerobic digestion phases removed NPE, regardless of whether TH pretreatment occurred. This research indicates that changes in biosolids processing can have impacts beyond just gas production and solids destruction.     

城市污水处理厂污泥的好氧处理研究

为了实现污泥的稳定化、减量化和无害化,对城市污水处理厂的浓缩污泥和厌氧消化污泥进行了好氧处理试验研究.试验结果表明,污泥好氧处理使污泥中有机物质含量降低,臭味减小.厌氧污泥经好氧消化处理后,一方面使污泥得到稳定化和减量化;另一方面,可以把污泥中的致病菌杀死.污泥经好氧消化后沉降性能有明显提高,絮凝剂的加入使其脱水性能也得到一定的改善.     

Investigation of the sludge reduction mechanism in the anaerobic side-stream reactor process using several control biological wastewater treatment processes

To investigate the mechanism of sludge reduction in the anaerobic side-stream reactor (SSR) process, activated sludge with five different sludge reduction schemes were studied side-by-side in the laboratory. These are activated sludge with: 1) aerobic SSR, 2) anaerobic SSR, 3) aerobic digester, 4) anaerobic digester, and 5) no sludge wastage. The system with anaerobic SSR (system #2) was the focus of this study and four other systems served as control processes with different functions and purposes. Both mathematical and experimental approaches were made to determine solids retention time (SRT) and sludge yield for the anaerobic SSR process. The results showed that the anaerobic SSR process produced the lowest solids generation, indicating that sludge organic fractions degraded in this system are larger than other systems that possess only aerobic or anaerobic mode. Among three systems that involved long SRT (system #1, #2, and #5), it was only system #2 that showed stable sludge settling and effluent quality, indicating that efficient sludge reduction in this process occurred along with continuous generation of normal sludge flocs. This observation was further supported by batch anaerobic and aerobic digestion data. Batch digestion on sludges collected after 109 days of operation clearly demonstrated that both anaerobically and aerobically digestible materials were removed in activated sludge with anaerobic SSR. In contrast, sludge reduction in the aerobic SSR process or no wastage system was achieved by removal of mainly aerobically digestible materials. All these results led us to conclude that repeating sludge under both feast/fasting and anaerobic/aerobic conditions (i.e., activated sludge with anaerobic SSR) is necessary to achieve the highest biological solids reduction with normal wastewater treatment performance.     

Model-based evaluation of competition between polyphosphate- and glycogen-accumulating organisms

Many studies show that glycogen-accumulating non-polyphosphate organisms (GAOs) can compete with polyphosphate-accumulating organisms (PAOs) for organic substrate under anaerobic conditions and may indeed cause the deterioration of enhanced biological phosphorus removal (EBPR) systems. Understanding their behaviors in an anaerobic/aerobic (A/O) system at different operational conditions is essential in developing control strategies that ensure EBPR. A model-based evaluation of competition between PAOs and GAOs under different operational conditions was presented in this study. At 30 degrees C and a 10-day sludge age, the dominance of GAOs in the A/O sequencing batch reactor (SBR) was strongly dependent upon their considerable kinetic advantage in anaerobic acetate uptake. At 20 degrees C and a 10-day sludge age, the kinetic advantage of GAOs in anaerobic acetate uptake could be less, compared to that at 30 degrees C and a 10-day sludge age, leading to the relative dominance of PAOs and a stable phosphorus removal in the A/O system. At 30 degrees C and a 3-day sludge age, the parameters responsible for determining the aerobic distribution of anaerobically stored X(PHA) for both PAOs and GAOs, other than kinetic parameters of anaerobic acetate uptake, are important for them being dominant in the A/O SBR. In a situation when the q(PHA,P) value is lower than q(PHA,G) but comparable, PAOs may still be dominant in the A/O SBR, presumably because their aerobic conversion fraction of biomass production from PHA was higher than that of the GAOs.     

Biodegradability of activated sludge organics under anaerobic conditions

From an experimental and theoretical investigation of the continuity of activated sludge organic (COD) compounds along the link between the fully aerobic or N removal activated sludge and anaerobic digestion unit operations, it was found that the unbiodegradable particulate organics (i) originating from the influent wastewater and (ii) generated by the activated sludge endogenous process, as determined from response of the activated sludge system, are also unbiodegradable under anaerobic digestion conditions. This means that the activated sludge biodegradable organics that can be anaerobically digested can be calculated from the active fraction of the waste activated sludge based on the widely accepted ordinary heterotrophic organism (OHO) endogenous respiration/death regeneration rates and unbiodegradable fraction. This research shows that the mass balances based steady state and dynamic simulation activated sludge, aerobic digestion and anaerobic digestion models provide internally consistent and externally compatible elements that can be coupled to produce plant wide steady state and dynamic simulation WWTP models.     

合成与实际污水中聚磷菌厌氧代谢研究

以实际生活污水为进水，在实验室对连续流A／O除磷系统进行了聚磷菌的驯化与培养，当系统对磷的去除率稳定在95％以上时利用烧杯批式试验考察了合成污水与实际污水中聚磷菌的厌氧代谢过程，并基于生物除磷的Mumleitner代谢模型，根据试验数据推求了表征聚磷菌厌氧代谢特性的化学计量参数及反应速率。结果表明，合成污水与实际污水中聚磷菌厌氧代谢过程生成的聚β羟基链烷酸的成分及反应速率存在显著差异，研究结果对采用活性污泥数学模型准确模拟实际污水中的生物除磷过程具有一定的参考价值。     

Endogenous processes during long-term starvation in activated sludge performing enhanced biological phosphorus removal

In many biological wastewater treatment systems, bacterial growth and the amount of active biomass are limited by the availability of substrate. Under these low growth conditions, endogenous processes have a significant influence on the amount of active biomass and therefore, the overall system performance. In enhanced biological phosphorus removal (EBPR) systems endogenous processes can also influence the levels of the internal storage compounds of the polyphosphate accumulating organisms (PAO), directly affecting phosphorus removal performance. The purpose of this study was to evaluate the significance of different endogenous processes that occur during the long-term starvation of EBPR sludge under aerobic and anaerobic conditions. Activated sludge obtained from a laboratory sequencing batch reactor was used to perform a series of batch starvation experiments. Under aerobic starvation conditions we observed a significant decay of PAO (first-order decay rate of 0.15/d) together with a rapid utilization of polyhydroxyalkanoates (PHA) and a slower utilization of glycogen and polyphosphate to generate maintenance energy. On the other hand, anaerobic starvation was best described by maintenance processes that rapidly reduce the levels of polyphosphate and glycogen under starvation conditions while no significant decay of PAO was observed. The endogenous utilization of glycogen for maintenance purposes is currently not included in available EBPR models. Our experimental results suggest that mathematical models for in EBPR should differentiate between aerobic and anaerobic endogenous processes, as they influence active biomass and storage products differently.     

Occurrence and behaviour of linear alkylbenzenesulphonates, nonylphenol, nonylphenol mono- and nonylphenol diethoxylates in sewage and sewage sludge treatment

The fluxes of linear alkylbenzenesulphonates (LAS), nonylphenol (NP), nonylphenol monoethoxylate (NP1EO) and nonylphenol diethoxylate (NP2EO) through sewage and sludge treatment of 29 Swiss sewage treatment plants were investigated. Reversed-phase high-performance liquid chromatography (HPLC) was used to determine LAS. Normal-phase HPLC was employed to measure NP, NP1EO and NP2EO which are metabolites of the nonionic surfactants of the nonylphenol polyethoxylate type (NPnEO). Quantitative determinations were performed of raw sewage, primary and secondary effluents and of sewage sludge. Under normal conditions of sewage and sludge treatment, LAS were efficiently removed from the raw wastewater (> 99% w/w) and were partly transferred to the sewage sludge (15–20% w/w). About 50% (molar base) of NPnEO in the sewage were transformed to NP and accumulated in the digested sludge. Large variations existed among different sewage treatment plants. It was estimated that 1.0 g m⁻² y⁻¹ of LAS and 0.3 g m⁻² y⁻¹ of NP are applied with sewage sludge to Swiss soils.     

Effect of long term anaerobic and intermittent anaerobic/aerobic starvation on aerobic granules

The effect of long term anaerobic and intermittent anaerobic/aerobic starvation on the structure and activity of aerobic granules was studied. Aerobic granular sludge treating abattoir wastewater and achieving high levels of nutrient removal was subjected to 4-5 week starvation under anaerobic and intermittent anaerobic/aerobic conditions. Microscopic pictures of granules at the beginning of the starvation period presented a round and compact surface morphology with a much defined external perimeter. Under both starvation conditions, the morphology changed at the end of starvation with the external border of the granules surrounded by floppy materials. The loss of granular compactness was faster and more pronounced under anaerobic/aerobic starvation conditions. The release of Ca²⁺ at the onset of anaerobic/aerobic starvation suggests a degradation of extracellular polymeric substances. The activity of ammonia oxidizing bacteria was reduced by 20 and 36% during anaerobic and intermittent anaerobic/aerobic starvation, respectively. When fresh wastewater was reintroduced, the granules recovered their initial morphology within 1 week of normal operation and the nutrient removal activity recovered fully in 3 weeks. The results show that both anaerobic and intermittent anaerobic/aerobic conditions are suitable for maintaining granule structure and activity during starvation.     

Decolorizing and detoxifying textile wastewater, containing both soluble and insoluble dyes, in a full scale combined anaerobic/aerobic system

The wastewater originating from the bleaching and dyeing processes in the textile factory Ten Cate Protect in Nijverdal (the Netherlands) was successfully treated in a sequential anaerobic/aerobic system. In the system, a combination of an anaerobic 70-m3 fluidized bed reactor and a 450-m3 aerobic basin with integrated tilted plate settlers, 80-95% of the color was removed. The color was largely removed in the preacidification basin and the anaerobic reactor. Color, deriving from both reactive as well as disperse, was anaerobically removed, indicating that these type of dyes were reduced to colorless products. Interestingly, the vat dyes, the anthraquinones and indigoids, which were thought to be removed mainly aerobically, were largely anaerobically decolorized. Apparently the anaerobic system is capable of effectively removing the color of both soluble as insoluble dyes. The treated effluent of the sequential anaerobic/aerobic treatment showed no toxicity towards the bioluminescent bacterium Vibrio fisheri (EC20 (95%) > 45%). Partially bypassing the anaerobic stage resulted in increased toxicity (EC20 (95%) of 9% and 14%) in the effluent of the aerobic treatment and caused significant decrease of color removal. The results of this study show a main contribution of anaerobic treatment in decolorizing and detoxifying the textile wastewater in the sequential anaerobic/aerobic system.     

Occurrence and fate of quinolone and fluoroquinolone antibiotics in a municipal sewage treatment plant

This study developed a method for analysis of nineteen quinolone and fluoroquinolone antibiotics (FQs) in sludge samples, and investigated the occurrence and fate of the FQs in a municipal sewage treatment plant (STP) with anaerobic, anoxic, and aerobic treatment processes. Eleven compounds, including pipemidic acid, fleroxacin, ofloxacin, norfloxacin, ciprofloxacin, enrofloxacin, lomefloxacin, sparfloxacin, gatifloxacin, moxifloxacin, and sarafloxacin (only in sludge), were detected in the STP. The predominance of ofloxacin and norfloxacin, followed by lomefloxacin, ciprofloxacin, gatifloxacin, and moxifloxacin, were found in wastewater, suspended solids, and sludge. The total concentrations of FQs were 2573 ± 241 ng/L, 1013 ± 218 ng/L, and 18.4 ± 0.9 mg/kg in raw sewage, secondary effluent, and sludge, respectively. Extremely low mass change percentages were observed for FQs in anaerobic, anoxic, and aerobic treatment units, suggesting biodegradation to be of minor importance in the removal of FQs in STPs. 50-87% of the initial FQs loadings (except for pipemidic acid (36%)) were ultimately found in the dewatered sludge. Mean removal efficiencies of FQs in the STP were 56-75%, except for new generation drugs such as moxifloxacin (40 ± 5%) and gatifloxacin (43 ± 13%). A significant positive correlation was found between removal efficiencies and K_d of FQs. The major factor in the removal of FQs in the STP was sorption to sludge, which was not governed by hydrophobic interactions. The long-term cycling and persistence of FQs in the STP has made activated sludge as a huge reservoir of FQ antibiotics.     

Removal of estrogenicity in Swedish municipal sewage treatment plants

The human estrogen receptor alpha-test, hosted in a yeast strain, was used to quantify estrogenicity in three-week composite samples of untreated and treated effluents from 20 Swedish municipal sewage treatment plants. The treatment plants were selected to represent different treatment processes regarding chemical precipitation and microbial procedures. The discharge from Swedish domestic sewage treatment plants contained estrogenic compounds corresponding to <0.1-15 ng estradiol equivalents/L. Low levels of estrogenic activity were also found in a river receiving municipal effluents, 3.5-35 km downstream the outlet from a sewage treatment works. The range of estrogenicity in untreated, raw sewage effluents was found to be 1-30 ng estradiol equivalents/L. Generally, wastewater treatment reduced the estrogenicity and extended biological treatment was most effective in its removal. Activated sludge treatment tended to be more effective than trickling filters, whereas chemical precipitation using iron or aluminium salts without biological treatment showed little effectivity. The study showed that treatment methods in current use are able to eliminate or largely reduce estrogenicity in domestic wastewater.     

Could polyphosphate-accumulating organisms (PAOs) be glycogen-accumulating organisms (GAOs)?

Polyphosphate (poly-P) is known to be a key compound in the metabolism of polyphosphate-accumulating organisms (PAOs). In this study, a sludge highly enriched (80%) in Candidatus Accumulibacter phosphatis (hereafter referred to as Accumulibacter), a widely known PAO, was used to study the ability of these microorganisms to utilize acetate anaerobically under poly-P-limiting conditions. The biomass was subject to several anaerobic and aerobic cycles, during which the poly-P pool of PAOs was gradually emptied by supplying feed deficient in phosphate and washing the biomass at the end of each anaerobic period using media containing no phosphorus. After three cycles, phosphorus was hardly released but PAOs were still able to take up acetate and stored it as polyhydroxyalkanoates (PHA), as demonstrated by post-FISH chemical staining. Glycogen degradation increased substantially, suggesting PAOs were using glycogen as the main energy source. This is a key feature of glycogen-accumulating organisms (GAOs), which are known to compete with PAOs in enhanced biological phosphorus removal (EBPR) systems. The ratios between acetate uptake, polyhydroxybutyrate (PHB) and polyhydroxyvalerate (PHV) production, and glycogen consumption agree well with the anaerobic models previously proposed for GAOs.     

Reduction of endocrine disruptor emissions in the environment: The benefit of wastewater treatment

The occurrence and fate of four estrogens and five alkylphenolic compounds were studied in thirteen plants with various treatment processes, sizes and countries. Complete load mass balance, including water and sludge phases, has shown a high reduction of the total load of hormones, around 90%. The removal of alkylphenols was more variable, due to the degradation of nonylphenol (NP) precursors - alkylphenol polyethoxylates (APnEO) - during the treatment, resulting in significant production of shorter and toxic alkylphenols (NP and short polyethoxylates) that concentrate in the sludges. Under anaerobic conditions, such as anaerobic digestion process, the load of NP was in most cases observed to increase. When considering the environmental impact, the high reduction of endocrine disrupting compounds (EDC) concentrations between raw wastewater and effluent enables to satisfy the requirements of the Water Framework Directive for NP except in very critical situations where the dilution factor of the effluent in the river would be lower than 7. For sludges, the pending European Directive on spreading of sludge on land would be complied with in all cases.     

Isolation, identification and utilization of thermophilic strains in aerobic digestion of sewage sludge

Two representative thermophilic bacterial strains (T1 and T2) were isolated from a one-stage autothermal thermophilic aerobic digestion pilot-scale reactor. 16S rRNA gene analysis indicated that they were Hydrogenophilaceae and Xanthomonodaceae. These isolated strains were inoculated separately and/or jointly in sewage sludge, to investigate their effects on sludge stabilization under thermophilic aerobic digestion condition. Four digestion conditions were tested for 480 h. Digestion without inoculation and inoculation with strain T2, as well as joint- inoculation with strains T1 and T2, achieved 32.6%, 43.0%, and 38.2% volatile solids (VS) removal, respectively. Removal in a digester inoculated with stain T1 only reached 27.2%. For the first 144 h, the three inoculated digesters all experienced higher VS removal than the digester without inoculations. Both specific thermophilic strains and micro-environment significantly affected the VS removal. DGGE profiles revealed that the isolated strains T1 and T2 can successfully establish in the thermophilic digesters. Other viable bacteria (including anaerobic or facultative microbes) also appeared in the digestion system, enhancing the microbial activity.     

Degradation of nonylphenolic surfactants in activated sludge batch tests

The fate of nonylphenol polyethoxylate surfactants in the activated sludge wastewater treatment process is a concern due to the formation of estrogenic nonlyphenols on degradation and due to the large amounts discharged to the aquatic environment through sewage treatment works. Batch tests using activated sludge from a Husmann apparatus were used to determine the effects of these compounds physico-chemical properties and biological sludge characteristics on biodegradation. Degradation of nonylphenol polyethoxylates with up to 12 ethoxy groups was observed in unacclimated sludge with a concomitant production of nonylphenol and short chain nonylphenol polyethoxylate compounds. Degradation was determined to be a biotic process involving intracellular enzyme activity, which resulted in sludge age being an influential parameter. With increasing sludge age there is an increase in mixed liquor solids concentration in activated sludge which results in greater bacterial numbers and the potential for greater species diversity which therefore increases compound degradation. However, increased degradation of long chain compounds resulted in an accumulation of shorter chain compounds and nonylphenol, which are more resistant to degradation.     

Development of granular sludge for textile wastewater treatment

Microbial granular sludge that is capable to treat textile wastewater in a single reactor under intermittent anaerobic and aerobic conditions was developed in this study. The granules were cultivated using mixed sewage and textile mill sludge in combination with anaerobic granules collected from an anaerobic sludge blanket reactor as seed. The granules were developed in a single sequential batch reactor (SBR) system under alternating anaerobic and aerobic condition fed with synthetic textile wastewater. The characteristics of the microbial granular sludge were monitored throughout the study period. During this period, the average size of the granules increased from 0.02 ± 0.01 mm to 2.3 ± 1.0 mm and the average settling velocity increased from 9.9 ± 0.7 m h⁻¹ to 80 ± 8 m h⁻¹. This resulted in an increased biomass concentration (from 2.9 ± 0.8 g L⁻¹ to 7.3 ± 0.9 g L⁻¹) and mean cell residence time (from 1.4 days to 8.3 days). The strength of the granules, expressed as the integrity coefficient also improved. The sequential batch reactor system demonstrated good removal of COD and ammonia of 94% and 95%, respectively, at the end of the study. However, only 62% of color removal was observed. The findings of this study show that granular sludge could be developed in a single reactor with an intermittent anaerobic-aerobic reaction phase and is capable in treating the textile wastewater.     

Combined anaerobic and aerobic digestion for increased solids reduction and nitrogen removal

A unique sludge digestion system consisting of anaerobic digestion followed by aerobic digestion and then a recycle step where thickened sludge from the aerobic digester was recirculated back to the anaerobic unit was studied to determine the impact on volatile solids (VS) reduction and nitrogen removal. It was found that the combined anaerobic/aerobic/anaerobic (ANA/AER/ANA) system provided 70% VS reduction compared to 50% for conventional mesophilic anaerobic digestion with a 20 day SRT and 62% for combined anaerobic/aerobic (ANA/AER) digestion with a 15 day anaerobic and a 5 day aerobic SRT. Total Kjeldahl nitrogen (TKN) removal for the ANA/AER/ANA system was 70% for sludge wasted from the aerobic unit and 43.7% when wasted from the anaerobic unit. TKN removal was 64.5% for the ANA/AER system.     

生物强化厌氧/好氧组合工艺处理模拟冰淇淋废水

从餐饮业下水道污泥中分离筛选出菌株B3，对模拟冰淇淋生产废水的厌氧水解过程进行生物强化，并考察其在厌氧阶段对COD去除率的影响及对后续好氧处理的影响。试验结果表明，经B3菌强化厌氧处理8h后对COD的去除率比未投菌的高31％，并有效促进了后续的好氧处理，尤其是对NH3-N的去除率提高了约40％，说明该菌具有很强的硝化功能。