Effects of polyvinylchloride microplastics on the toxicity of nanoparticles and antibiotics to aerobic granular sludge: Nitrogen removal, microbial community and resistance genes.

Copper oxide nanoparticles (CuO NPs) and ciprofloxacin (CIP) have ecological risk to humans and ecosystems. Polyvinylchloride microplastics (PVC MPs), as a representative of microplastics, may often coexist with CuO NPs and CIP in wastewater treatment systems due to their widespread application. However, the co-impact of PVC MPs in wastewater systems contained with CuO NPs and CIP on nitrogen removal and ecological risk is not clear. In this work, PVC MPs co-impacts on the toxicity of CuO NPs and CIP to aerobic granular sludge (AGS) systems and potential mechanisms were investigated. 10 mg/L PVC MPs co-addition did not significantly affect the nitrogen removal, but it definitely changed the microbial community structure and enhanced the propagation and horizontal transfer of antibiotics resistance genes (ARGs). 100 mg/L PVC MPs co-addition resulted in a raise of CuO NP toxicity to the AGS system, but reduced the co-toxicity of CuO NPs and CIP and ARGs expression. The co-impacts with different PVC MPs concentration influenced Cu2+ concentrations, cell membrane integrity, extracellular polymeric substances (EPS) contents and microbial communities in AGS systems, and lead to a change of nitrogen removal.

Rapid start-up of partial nitrification reactor by exogenous AHLs and Vanillin combined with intermittent aeration.

Quorum sensing (QS) and quorum quenching (QQ) are common phenomena in microbial systems and play an important role in the nitrification process. However, rapidly start up partial nitrification regulated by N-acyl-homoserine lactones (AHLs)-mediated QS or QQ has not been reported. Hence, we chose N-butyryl homoserine lactone (C4-HSL) and N-hexanoyl homoserine lactone (C6-HSL) as the representative AHLs, and Vanillin as the representative quorum sensing inhibitor (QSI) combined intermittent aeration to investigate their effects on the start-up process of partial nitrification. The start-up speed in the group with C4-HSL or C6-HSL addition was 1.42 or 1.26 times faster than that without addition, respectively. Meanwhile, the ammonium removal efficiency with C4-HSL or C6-HSL addition was increased by 13.87 % and 17.30 % than that of the control group, respectively. And, partial nitrification could maintain for a certain period without AHLs further addition. The increase of Nitrosomonas abundance and ammonia monooxygenase (AMO) activity, and the decrease of Nitrobacter abundance and nitrite oxidoreductase (NXR) activity were the reasons for the rapid start-up of partial nitrification in the AHLs groups. Vanillin addition reduced AMO and hydroxylamine oxidoreductase (HAO) activity, and increased Nitrobacter abundance and NXR activity, thus these were not conducive to achieving partial nitrification. Denitrifying bacteria (Hydrogenophaga, Thauera and Aquimonas) abundance increased in the Vanillin group. QS-related bacteria and gene abundance were elevated in the AHLs group, and reduced in the Vanillin group. Function prediction demonstrated that AHLs promoted the nitrogen cycle while Vanillin enhanced the carbon cycle. This exploration might provide a new technical insight into the rapid start-up of partial nitrification based on QS control.

Co-existence effect of copper oxide nanoparticles and ciprofloxacin on simultaneous nitrification, endogenous denitrification, and phosphorus removal by aerobic granular sludge.

Nanoparticles and antibiotics are toxic to humans and ecosystems, and they inevitably coexist in the wastewater treatment plants. Hence, the co-existence effects and stress mechanism of copper (II) oxide nanoparticles (CuO NPs) and ciprofloxacin (CIP) on simultaneous nitrification, endogenous denitrification and phosphorus removal (SNEDPR) by aerobic granular sludge (AGS) were investigated here. The co-existence stress of 5 mg/L CuO NPs and 5 mg/L CIP resulted in the synergistic inhibitory effect on nutrient removal. Transformation inhibition mechanisms of carbon (C), nitrogen (N) and phosphorus (P) with CuO NPs and CIP addition were time-dependent. Furthermore, the long-term stress mainly inhibited PO43--P removal by inhibiting phosphorus release process, while short-term stress mainly inhibited phosphorus uptake process. The synergistic inhibitory effect of CuO NPs and CIP may be due to the changes of physicochemical characteristics under the co-existence of CuO NPs and CIP. This further altered the sludge characteristics, microbial community structure and functional metabolic pathways under the long-term stress. Resistance genes analysis exhibited that the co-existence stress of CuO NPs and CIP induced the amplification of qnrA (2.38 folds), qnrB (4.70 folds) and intI1 (3.41 folds) compared with the control group.

Short-term responses of the anammox process to Ni(II): nitrogen removal, mechanisms and inhibition recovery.

Anaerobic ammonia oxidizing (anammox) has already been recognized as an innovative and economical nitrogen removal technology. However, the effect of heavy metals on anammox bacteria in aquatic ecosystem remains largely unknown. Ni(II) is a common kind of heavy metals detected in industrial wastewater and municipal sewage treatment plants. Hence, the responses of the anammox process to Ni(II) were studied here. The results showed that anammox was the dominant reaction with Ni(II) concentrations no more than 25 mg/L. 1 mg/L of Ni(II) addition promoted nitrogen removal by anammox. The higher the Ni(II) concentrations and longer exposure time, the more inhibition for anammox bacteria was gotten. The IC50 of Ni(II) to anammox was determined as 83.86 mg/L by an exponential regression equation. The inhibition of Ni(II) on anammox activity was mainly attributed to intracellular accumulation Ni(II) inhibition to HDH activity. Two times increase of IC50 after 4 times circles of domestication suggests multiple intermittent domestication can increase the tolerance of anammox bacteria to Ni(II). EDTA washing can eliminate the inhibition of anammox activity by Ni(II) with Ni(II) addition no more than 25 mg/L.

[Effect of Ni(â ¡) on Anaerobic Ammonium Oxidation and Changes in Kinetics].

Anaerobic ammonium oxidation (ANAMMOX) is widely used for treatment of ammonium-rich wastewater because of its economic and environmental benefits. However, ANAMMOX bacteria are sensitive to environmental conditions, especially to heavy metals. The short-term and long-term effects of Ni(Ⅱ) on ANAMMOX were studied by batch and continuous flow experiments, respectively. Results showed that low concentrations of Ni(Ⅱ) had promoted nitrogen removal by ANAMMOX and high concentrations inhibited ANAMMOX performance during a short-term period. Compared with the specific anaerobic ammonium oxidation activity (SAA) without Ni(Ⅱ) addition, SAA with 1 mg·L-1 Ni(Ⅱ) addition increased by 11.14% and the SAA with 100 mg·L-1 Ni(Ⅱ) addition reduced by 49.55%. The IC50 of Ni(Ⅱ) for ANAMMOX was determined to be 83.86 mg·L-1. In contrast, long-term Ni(Ⅱ) addition significantly suppressed nitrogen removal of ANAMMOX, and the suppression threshold of Ni(Ⅱ) on ANAMMOX was 15 mg·L-1. The Monod model was applied to simulate the kinetics of ANAMMOX without Ni(Ⅱ) addition. The qmax0(TN/VSS) and KS0 values were 12.25 mg·(g·h)-1 and 405.36 mg·L-1, respectively. The modified Haldane model was suitable to describe the kinetics of ANAMMOX with 50 mg·L-1 Ni(Ⅱ) addition. The qmax(TN/VSS), KS, and Ki values were 6.78 mg·(g·h)-1, 313.2 mg·L-1, and 1.32, respectively. The inhibition of ANAMMOX by Ni(Ⅱ) is anticompetitive inhibition. In addition, the inhibition of Ni(Ⅱ) on ANAMMOX was mainly related to the content of intracellular Ni(Ⅱ). The IC50intracellular Ni(Ⅱ)(VSS) of intracellular Ni(Ⅱ) was 0.072 mg·g-1.

17 beta-estradiol biodegradation by anaerobic granular sludge: Effect of iron sources.

Steroid estrogens, as typical endocrine disrupting chemicals (EDCs), have raised an increasing concern due to their endocrine disrupting effects on aquatic animals and potential hazards on human health. Batch experiments were conducted to study 17 beta-estradiol (E2) removal and Estradiol Equivalent Quantity (EEQ) elimination by anaerobic granular sludge (AnGS) combined with different valence iron sources. Results showed that E2 was effectively biodegraded and transformed into E1 by AnGS. The addition of different valence iron sources all promoted E2 degradation, reduced E2 Equivalent Quotient (EEQ) concentration, and increased methane production in the batch experiments. The enhancement effect of zero-valent iron (ZVI) on E2 removal and EEQ elimination was stronger than that of Fe2+ and Fe3+ in our experiments. The enhancement effect proportion of ZVI corrosion, Fe2+, and Fe3+ in the process of E2 degradation by AnGS combined with ZVI were 42.26%, 40.21% and 17.53%, respectively.

Long-term effects of N-acyl-homoserine lactone-based quorum sensing on the characteristics of ANAMMOX granules in high-loaded reactors.

Laboratory experiments were carried out to determine the long-term effects of N-acyl-homoserine lactone (AHL)-based quorum sensing on the characteristics of ANAMMOX granules in high-loaded reactors. Results clearly showed that adding 30 mg L-1 N-octanoyl-DL-homoserinelactone (C8-HSL) at the initial stage (1-40 d) of the experiment had long-term positive effects on the settleability of granules and controlled the sludge floatation effectively. C8-HSL decreased the content of bound extracellular polymeric substances (B-EPS) and the ratio of protein to carbohydrate (PN/PS) by 17% and 48%, respectively and increased the relative hydrophobicity (RH) of the granules by 28%. The results of batch tests indicated that C8-HSL significantly reduced the content of loosely-bound EPS (LB-EPS) in the B-EPS, which was responsible for variations in granule settleability and stability. Thus, the settleability of the granules was improved significantly due to addition of C8-HSL, contributing to operational stability and the high TN removal efficiency of the reactor. On day 150, when the nitrogen loading rates of all reactors were 13.4 kg TN m-3 d-1, the nitrogen removal rate and nitrogen removal efficiency of the reactor with C8-HSL (R3) were up to 11.2 kg TN m-3 d-1 and 88%, respectively. N-hexanoyl-DL-homoserine lactone (C6-HSL) improved activity of the granules, while N-dodecanoyl-DL-homoserine lactone (C12-HSL) had no effect on the characteristics of the granules. The long-term effects of C8-HSL on the settleability of granules may be attributed to sustainable release of endogenous signals induced by exogenous signal.

Inhibition factors and Kinetic model for ammonium inhibition on the anammox process of the SNAD biofilm.

The aim of the present work was to evaluate the anaerobic ammonium oxidation (anammox) activity of simultaneous partial nitrification, anammox and denitrification (SNAD) biofilm with different substrate concentrations and pH values. Kaldnes rings taken from the SNAD biofilm reactor were incubated in batch tests to determine the anammox activity. Haldane model was applied to investigate the ammonium inhibition on anammox process. As for nitrite inhibition, the NH4+-N removal rate of anammox process remained 87.4% of the maximum rate with the NO2--N concentration of 100mg/L. Based on the results of Haldane model, no obvious difference in kinetic coefficients was observed under high or low free ammonia (FA) conditions, indicating that ammonium rather than FA was the true inhibitor for anammox process of SNAD biofilm. With the pH value of 7.0, the rmax, Ks and KI of ammonium were 0.209kg NO2--N/kg VSS/day, 9.5mg/L and 422mg/L, respectively. The suitable pH ranges for anammox process were 5.0 to 9.0. These results indicate that the SNAD biofilm performs excellent tolerance to adverse conditions.

Effects of carbon sources, COD/NO2--N ratios and temperature on the nitrogen removal performance of the simultaneous partial nitrification, anammox and denitrification (SNAD) biofilm.

The aim of the present work was to evaluate the effects of carbon sources and chemical oxygen demand (COD)/NO2--N ratios on the anammox-denitrification coupling process of the simultaneous partial nitrification, anammox and denitrification (SNAD) biofilm. Also, the anammox activities of the SNAD biofilm were investigated under different temperature. Kaldnes rings taken from the SNAD biofilm reactor were operated in batch tests to determine the nitrogen removal rates. As a result, with the carbon source of sodium acetate, the appropriate COD/NO2--N ratios for the anammox-denitrification coupling process were 1 and 2. With the COD/NO2--N ratios of 1, 2, 3, 4 and 5, the corresponding NO2--N consumption via anammox was 87.1%, 52.2%, 29.3%, 23.7% and 16.3%, respectively. However, with the carbon source of sodium propionate and glucose, the anammox bacteria was found to perform higher nitrite competitive ability than denitrifiers at the COD/NO2--N ratio of 5. Also, the SNAD biofilm could perform anammox activity at 15 °C with the nitrogen removal rate of 0.071 kg total inorganic nitrogen per kg volatile suspended solids per day. These results indicated that the SNAD biofilm process might be feasible for the treatment of municipal wastewater at normal temperature.

Inhibition kinetics of nitritation and half-nitritation of old landfill leachate in a membrane bioreactor.

Nitritation can be used as a pretreatment for anaerobic ammonia oxidation (anammox). Various control strategies for nitritation and half-nitritation of old landfill leachate in a membrane bioreactor were investigated in this study and the inhibition kinetics of substrate, product and old landfill leachate on nitritation were analyzed via batch tests. The results demonstrated that old landfill leachate nitritation in the membrane bioreactor can be achieved by adjusting the influent loading and dissolved oxygen (DO). From days 105-126 of the observation period, the average effluent concentration was 871.3 mg/L and the accumulation rate of [Formula: see text] was 97.2%. Half-nitritation was realized quickly by adjusting hydraulic retention time and DO. A low-DO control strategy appeared to best facilitate long-term and stable operation. Nitritation inhibition kinetic experiments showed that the inhibition of old landfill leachate was stronger than that of the substrate [Formula: see text] or product [Formula: see text] . The ammonia oxidation rate dropped by 22.2% when the concentration of old landfill leachate (calculated in chemical oxygen demand) was 1600.2 mg/L; further, when only free ammonia or free nitrous acid were used as a single inhibition factor, the ammonia oxidation rate dropped by 4.7-6.5% or 14.5-15.9%, respectively. Haldane, Aiba, and a revised inhibition kinetic model were adopted to separately fit the experimental data. The R2 correlation coefficient values for these three models were 0.982, 0.996, and 0.992, respectively.

A coupled system of half-nitritation and ANAMMOX for mature landfill leachate nitrogen removal.

A coupled system of membrane bioreactor-nitritation (MBR-nitritation) and up-flow anaerobic sludge blanket-anaerobic ammonium oxidation (UASB-ANAMMOX) was employed to treat mature landfill leachate containing high ammonia nitrogen and low C/N. MBR-nitritation was successfully realized for undiluted mature landfill leachate with initial concentrations of 900-1500 mg/L [Formula: see text] and 2000-4000 mg/L chemical oxygen demand. The effluent [Formula: see text] concentration and the [Formula: see text] accumulation efficiency were 889 mg/L and 97% at 125 d, respectively. Half-nitritation was quickly realized by adjustment of hydraulic retention time and dissolved oxygen (DO), and a low DO control strategy could allow long-term stable operation. The UASB-ANAMMOX system showed high effective nitrogen removal at a low concentration of mature landfill leachate. The nitrogen removal efficiency was inhibited at excessive influent substrate concentration and the nitrogen removal efficiency of the system decreased as the concentration of mature landfill leachate increased. The MBR-nitritation and UASB-ANAMMOX processes were coupled for mature landfill leachate treatment and together resulted in high effective nitrogen removal. The effluent average total nitrogen concentration and removal efficiency values were 176 mg/L and 83%, respectively. However, the average nitrogen removal load decreased from 2.16 to 0.77 g/(L d) at higher concentrations of mature landfill leachate.

Adsorptive removal of naphthalene induced by structurally different Gemini surfactants in a soil-water system.

A new generation of surfactant, Gemini surfactants, have been synthesized and have attracted the attention of various industrial and academic research groups. This study focused on the use of symmetric and dissymmetric quaternary ammonium Gemini surfactants to immobilize naphthalene onto soil particles, and is used as an example of an innovative application to remove HOC in situ using the surfactant-enhanced sorption zone. The sorption capacity of modified soils by Gemini surfactant and natural soils was compared and the naphthalene sorption efficiency, in the absence and presence of Gemini surfactants with different alkyl chain lengths, was investigated in the soil-water system. The results have shown that the increased added Gemini surfactant formed admicelles at the interface of soil/water having superior capability to retard contaminant. Symmetric and dissymmetric Gemini surfactants have opposite effect on the aspect of removing of PAH attributing to their solubilization and sorption behavior in soil-water system. Compared with the natural soil, sorption of naphthalene by Gemini-modified soil is noticeably enhanced following the order of C12-2-16 < C12-2-12 < C12-2-8. However, the symmetric Gemini surfactant C12-2-12 is the optimized one for in situ barrier remediation, which is not only has relative high retention ability but also low dosage.

Nitrogen removal via simultaneous partial nitrification, anammox and denitrification (SNAD) process under high DO condition.

The simultaneous partial nitrification, anammox and denitrification (SNAD) process for treating domestic wastewater was investigated in a sequencing batch reactor (SBR). The SBR was operated with air flow rate of 500 L h-1 at 30 °C. Domestic wastewater was used as influent and Kaldnes rings were used as biomass carriers. In the beginning, long aeration condition was implemented to cultivate nitrification biofilm. Afterwards, intermittent aerobic condition was conducted during the cycle operation. The influent organic matter loading rate was improved by reducing the aeration and mixing times. Consequently, when the SNAD biofilm reactor was fed with the organic matter loading rate of 0.77 (kg COD m-3 d-1), the bio-bubbles appeared in the reactor and the total inorganic nitrogen (TIN) removal efficiency decreased. After the organic matter loading rate decreased to 0.67 (kg COD m-3 d-1), the reactor showed excellent nitrogen removal performance. The TIN removal efficiency varied between 80 and 90 %, and the average TIN removal loading rate was 0.22 (kg TIN m-3 d-1). Additionally, the scanning electron microscope (SEM) observation confirmed that the anammox bacteria located in the inner part of the carriers. Finally, the microbial community analysis of 16S rRNA gene cloning revealed that the anammox bacteria on the carriers consisted of three main genuses: Candidatus Brocadia sp., Candidatus Brocadia caroliniensis and Candidatus Brocadia fulgida.

The nitritation performance of biofilm reactor for treating domestic wastewater under high dissolved oxygen.

The objective of this study was to investigate the nitritation performance in a biofilm reactor for treating domestic wastewater. The reactor was operated in continuous feed mode from phases 1 to 3. The dissolved oxygen (DO) was controlled at 3.5-7 mg/L throughout the experiment. The biofilm reactor showed excellent nitritation performance after the inoculation of nitrifying sludge, with the hydraulic retention time being reduced from 24 to 7 hr. Above 90% nitrite accumulation ratio (NAR) was maintained in phase 1. Afterwards, nitratation occurred with the low NH4(+)-N concentration in the reactor. The improvement of NH4(+)-N concentration to 20-35 mg/L had a limited effect on the recovery of nitritation. However, nitritation recovered rapidly when sequencing batch feed mode was adopted in phase 4, with the effluent NH4(+)-N concentration above 7 mg/L. The improvement of ammonia oxidizing bacteria (AOB) activity and the combined inhibition effect of free ammonia (FA) and free nitrous acid (FNA) on the nitrite oxidizing bacteria (NOB) were two key factors for the rapid recovery of nitritation. Sludge activity was obtained in batch tests. The results of batch tests had a good relationship with the long term operation performance of the biofilm reactor.

Microbial Internal Storage Alters the Carbon Transformation in Dynamic Anaerobic Fermentation.

Microbial internal storage processes have been demonstrated to occur and play an important role in activated sludge systems under both aerobic and anoxic conditions when operating under dynamic conditions. High-rate anaerobic reactors are often operated at a high volumetric organic loading and a relatively dynamic profile, with large amounts of fermentable substrates. These dynamic operating conditions and high catabolic energy availability might also facilitate the formation of internal storage polymers by anaerobic microorganisms. However, so far information about storage under anaerobic conditions (e.g., anaerobic fermentation) as well as its consideration in anaerobic process modeling (e.g., IWA Anaerobic Digestion Model No. 1, ADM1) is still sparse. In this work, the accumulation of storage polymers during anaerobic fermentation was evaluated by batch experiments using anaerobic methanogenic sludge and based on mass balance analysis of carbon transformation. A new mathematical model was developed to describe microbial storage in anaerobic systems. The model was calibrated and validated by using independent data sets from two different anaerobic systems, with significant storage observed, and effectively simulated in both systems. The inclusion of the new anaerobic storage processes in the developed model allows for more successful simulation of transients due to lower accumulation of volatile fatty acids (correction for the overestimation of volatile fatty acids), which mitigates pH fluctuations. Current models such as the ADM1 cannot effectively simulate these dynamics due to a lack of anaerobic storage mechanisms.

[Characteristic research of shortcut denitrification in synthetic ammonia industrial wastewater treatment process].

Active sludge was from a pilot-scale synthetic ammonia industrial wastewater treatment plant with a strengthen anoxic-oxic (A/O) technology. The zero order kinetic model was suit for describing shortcut and complete denitrification process. Experimental results showed that shortcut denitrification could reduce 14.1% carbon source consumption and 55.7% denitrification time, respectively, comparing with complete denitrification. The maximum specific denitrification rate was 0.509 g x (g x d)(-1) with an initial NO2(-) -N concentration of 36.82 mg x L(-1) and pH 7.5. In the industrial practice, it must be avoided pH higher than 9.0 in anoxic zone for industrial treatment. Replication-selective denitrifying bacteria showed a strong adaptability to methanol and ethanol, but showed maladaptation to other small molecular and easily biodegradable organics, such as glucose and acetic acid.

Modeling anaerobic digestion of aquatic plants by rumen cultures: cattail as an example.

Despite of the significance of the anaerobic digestion of lignocellulosic materials, only a limited number of studies have been carried out to evaluate the lignocellulosic digestion kinetics, and information about the modeling of this process is limited. In this work, a mathematical model, based on the Anaerobic Digestion Model No.1 (ADM1), was developed to describe the anaerobic conversion of lignocellulose-rich aquatic plants, with cattail as an example, by rumen microbes. Cattail was fractionated into slowly hydrolysable fraction (SHF), readily hydrolysable fraction (RHF) and inert fraction in the model. The SHF was hydrolyzed by rumen microbes and resulted in the production of RHF. The SHF and RHF had different hydrolysis rates but both with surface-limiting kinetics. The rumen microbial population diversity, including the cattail-, butyrate-, acetate- and H(2)-degraders, was all incorporated in the model structure. Experiments were carried out to identify the parameters and to calibrate and validate this model. The simulation results match the experimental data, implying that the fractionation of cattail into two biodegradation parts, i.e., SHF and RHF, and modeling their hydrolysis rate with a surface-limiting kinetics were appropriate. The model was capable of simulating the anaerobic biodegradation of cattail by the rumen cultures.