Intensifying the simultaneous removal of nitrogen and phosphorus of an integrated aerobic granular sludge-membrane bioreactor by Acinetobacter junii.

This work aims at intensifying the simultaneous removal of nitrogen and phosphorus of an integrated aerobic granular sludge (AGS) - membrane bioreactor (MBR) by Acinetobacter junii. After acclimation and enrichment in a sequencing batch reactor (SBR), Acinetobacter junii, a kind of denitrifying phosphate accumulating organism (DPAO), was successfully screened in the used SBR. Then it was verified to be capable of effectively enhancing the performance in the simultaneous removal of nitrogen and phosphorus of AGS-MBR. In the system, DPAO (Acinetobacter junii) mainly occurred in AGS, and the highest ratio even reached 22.8%, but its competitive advantages highly depend on the size of AGS. The presented results can cultivate AGS and enrich DPAO simultaneously to improve the removal of nitrogen and phosphorus of an AGS-MBR, which provide an environmentally friendly approach to upgrade traditional wastewater treatment processes.

Ecological risk assessment of the typical anti-epidemic drugs in the Pearl River Delta by tracing their source and residual characteristics.

Since the outbreak of the COVID-19 pandemic, the anti-epidemic drugs have been used in extraordinary quantities with high intensity, and concerns have grown about their potential ecological risks due to their continued release and persistence in the receiving environments. A systematic investigation, covering the samples from hospital wastewater, effluent from wastewater treatment plants and receiving water bodies in the Pearl River Delta Region (PRDR), was carried out and aimed at tracing the sources and fate of 30 typical anti-epidemic in different water matrixes and evaluating their ecological risk. The results showed that these typical anti-epidemic drugs residues were detected in most of the sampling sites, with the highest concentration measured in hospital wastewater, whose concentrations were as high as ppb level, while the highest concentration of the surface water samples in tributaries was lower than ppb level. Anti-epidemic drugs contained in hospital wastewater and effluent from WWTPs were the main sources of drug residues in the surface water of this region. In the surface water of PRDR, although the detected concentration anti-epidemic drugs were basically in the range of 0-10 ng/L. The risk quotient of several anti-epidemic drugs, including Ciprofloxacin (CFX), Ofloxacin (OFX), Erythromycin (ETM), Clindamycin (CLI), and Sulfamethoxazole (SMX), was calculated to be a high value, which indicated that they might cause non-negligible ecological risk to the aquatic environment.

Insights into the life-cycle of aerobic granular sludge in a continuous flow membrane bioreactor by tracing its heterogeneous properties at different stages.

This work gave insights into the life-cycle of aerobic granular sludge (AGS) by tracing its heterogeneity in the basic properties at different stages in a closed system (a continuous flow membrane bioreactor, MBR), including physical and chemical characteristics and microbial communities. The results indicate that the entire life-cycle consists of the following four stages, namely, the initial, growing, mature and cleaved stages, where multiple AGS properties synergistically affect the rheological properties of the AGS over its life-cycle. The storage modulus (G') of AGS reached its maximum value at the mature stage, whose value was significantly and positively correlated with the protein (PN) in extracellular polymeric substances (EPS) and granule size, specifically the peak area of granule size distribution, but this value was strongly and negatively correlated with the roughness. The AGS at the mature stage would be more vulnerable to be destroyed than that at other stages under the condition of higher shear strain, such as γ = 50%, which was associated with larger granule size and fewer polysaccharide (PS)-related functional groups (especially in the soluble microbial products (SMPs) in the outermost layer of AGS), and the decrease in PS was correlated with a higher relative abundance of Chloroflexi. Additionally, the value of shear strain that AGS was subjected to had a good linear correlation (R2=0.993) with the Young's modulus, which indicated the ability of AGS to resist deformation improved with increasing values of shear strain.

Spectral change of dissolved organic matter after extracted by solid-phase extraction and its feasibility in predicting the acute toxicity of polar organic pollutants in textile wastewater.

Spectroscopic parameters can be used as proxies to effectively trace the occurrence of organic trace contaminants, but their suitability for predicting the toxicity of discharged industrial wastewater with similar spectra is still unknown. In this study, the organic contaminants in treated textile wastewater were subdivided and extracted by four commonly-used solid-phase extraction (SPE) cartridges, and the resulting spectral change and toxicity of textile effluent were analyzed and compared. After SPE, the spectra of the percolates from the four cartridges showed obvious differences with respect to the substances causing the spectral changes and being more readily adsorbed by the WAX cartridges. Non-target screening results showed source differences in organic micropollutants, which were one of the main contributors leading to their spectral properties and spectral variations after SPE in the effluents. Two fluorescence parameters (C1 and humic-like) identified by the excitation emission matrix-parallel factor analysis (EEM-PARAFAC) were closely correlated to the toxicity endpoints for Scenedesmus obliquus (inhibition ratios of cell growth and Chlorophyll-a synthesis), which can be applied to quantitatively predict the change of toxicity effect caused by polar organic pollutants. The results would provide novel insights into the spectral feature analysis and toxicity prediction of the residual DOM in industrial wastewater.

Distribution characteristics of phosphorus-containing substances in a long running aerobic granular sludge-membrane bioreactor with no sludge discharge.

This work aimed at revealing the distribution characteristics of phosphorus (P) containing substances in an aerobic granular sludge-membrane bioreactor (AGS-MBR). During the long running period (180 days) with no sludge discharge, AGS was successfully cultivated on day 20, and the system performed well in removing organic pollutants and total nitrogen (TN). However, the removal of total P (TP) showed a fluctuant tendency, and P was found to distribute in all the phases of the system. In the intracellular phase, it occupied the largest ratio all through the period. In AGS, inorganic P (IP) was measured to be about 74.4-77.8% of TP, with non-apatite IP (NAIP) composing 57.5-69.6%, while in organic P (OP), the ratio of monoester and diester phosphate was in the range of 19-26.9% and 12-13.5%, respectively. The presence of highly releasable and bioavailable P (NAIP + OP) in AGS implied that it might be a potential P resource for utilization.

Towards deep purification of secondary textile effluent by using a dynamic membrane process: Pilot-scale verification.

The present investigation used regular powered activated carbon (PAC) as the dynamic membrane (DM) material and successfully built-up a pilot-scale DM system for deep purification of the secondary textile effluent, which aimed at verifying the technical and economic feasibility of the DM with real secondary textile effluent. The hydrodynamic experiments indicated that the filtration resistance gradually increased along with the operation of DM system, and among which, the PAC size was the most important influencing factor. More dosage and smaller sized PAC were beneficial to enhance the purification effect of micro-organic pollutants, but they simultaneously improved the operational costs, which implied that the adoption of DM materials should comprehensively consider the removal results and the type and dosage of DM materials for obtaining an optimal result, and the operational costs would be drastically reduced by regenerating the wasted PAC. More than 50% residual micro-organic pollutants were further removed by the system, and they were mainly some aliphatic and aromatic compounds, which were the main refractory organic pollutants in most textile effluents. It was also proved by the pilot-scale DM study that the removed residual pollutants from the secondary textile effluent were mainly aromatic protein II. Due to the contained complex functional groups in their molecular structure, soluble microbial metabolites were relatively easier to be removed by the DM layer.

Rapid granulation of aerobic granular sludge and maintaining its stability by combining the effects of multi-ionic matrix and bio-carrier in a continuous-flow membrane bioreactor.

The present investigation aimed at providing a novel approach to promote the rapid granulation and stability of aerobic granular sludge (AGS) in a continuous-flow membrane bioreactor (MBR). By operating two identical MBRs with or with no bio-carrier for 125 days, it was found that the combination of multi-ionic matrix and bio-carrier could promote the rapid formation and maintain the long-term stability of AGS. The primary AGS was first observed inside the reactor on day 14, and the mature AGS appeared soon and kept stable for more than 4 months (its average size still was about 800 µm on day 125). Suitable filling ratio of bio-carrier was beneficial to form a stable and regular circulating water flow inside, and adding divalent metal ions quickly reduced the negative charges of tiny sludge particles, which were two essential factors leading to the rapid granulation of AGS and maintaining its stability. The multi-ionic matrix not only enhanced the biological aggregation process, but also facilitated the expansion of the cultivated AGS into a new multi-habitat system of Mn-AGS, in which, complex microbial communities with rich bio-diversity robustly promoted the efficient removal of organic pollutants and nutrients.

Insights into the fouling layer of flat-sheet membrane and its development in an integrated oxidation ditch-membrane bioreactor.

This work revealed the characteristics of fouling layer on the flat-sheet membranes and its development in an integrated oxidation-ditch membrane bioreactor. During the operation period (130 days), the reactor performed very well in removing pollutants. As the operation proceeded, membrane fouling occurred on the flat-sheet membranes and trans-membrane pressure showed a cyclical variation. The experimental results showed that the process of membrane fouling appeared successively in two different structures: biofilm (BF) and sludge fouling (SF). The substances causing membrane fouling were mainly organic foulants and a small amount of inorganic metal compounds, especially the protein-like and fulvic acid-like substances in loosely bound extracellular polymeric substances (LB-EPS). The analysis of microbial communities revealed that SF and BF had very different microbial properties. Although most membrane foulants could be removed by physical and chemical cleaning methods, the protein-like and fulvic acid-like substances in BF were contribute much to causing irreversible membrane fouling.

Tracing the occurrence of organophosphate ester along the river flow path and textile wastewater treatment processes by using dissolved organic matters as an indicator.

Organophosphate esters (OPEs) are frequently detected in wastewater and receiving river, but their occurrence is hard to be quickly and effectively responded. In this study, the relevant OPEs and dissolved organic matters (DOMs) data were obtained from two textile wastewater treatment plants (WWTPs) with different processes and a 15 km stretch of river receiving the treated textile wastewater. UV-Vis absorption and fluorescence spectroscopy combined with peak-picking and fluorescence regional integration (FRI) methods were used to characterize DOM components in these samples. The results showed that OPEs concentrations were not always consistent with that of DOM, but were related to their physico-chemical properties and sources. Correlation and regression analysis indicated that the FRI pattern could be considered for tracing the occurrence of organophosphate diesters derived from multiple pollutants in river water, and reflected the emerging of moderate or high removal organophosphate triesters in WWTPs. Difference in the sources and DOM compositions was the main contributor to the correlation difference of OPEs and DOM in the two types of processes. The treatment technique also played important roles in the co-occurrence of OPEs and DOM in different WWTPs. This study would be beneficial to develop in-situ monitoring for the dynamic change of emerging contaminants along with a river flow path and from WWTPs, respectively.

Occurrence, ecotoxicological risks of sulfonamides and their acetylated metabolites in the typical wastewater treatment plants and receiving rivers at the Pearl River Delta.

Sulfonamides (SAs) were frequently detected in various environmental water bodies because of their incomplete removal during wastewater treatment process, and this may lead to a negative effect on aquatic ecosystems. This study investigated six SAs and three of their acetylated metabolites in the influents, effluents, and the receiving river waters from four typical wastewater treatment plants (WWTPs) at the Pearl River Delta in Guangdong province, China. The results indicated that sulfadiazine, sulfapyridine and sulfamethoxazole had the highest detection frequency. Moreover, sulfadiazine and sulfamethoxazole had its maximum concentrations (216 ng/L and 200 ng/L, respectively) in the influent during dry season. To evaluate the compound degradability, the removal efficiency of each individual sulfonamide was calculated, and a modified method to assess it was recommended considering the widespread inter-conversion between SAs and their metabolites. Finally, regarding the effluent and river water, potential environmental risk based on the Hazard quotients (HQs) was estimated towards three diverse non-targeted organisms. Sulfamethoxazole was assessed with the highest HQ (>3.6), being the sole sulfonamide that would pose a risk to algae in the effluents and river waters. Thus, SAs emission needs to be further reduced from WWTPs into the environment.

Promoting the granulation process of aerobic granular sludge in an integrated moving bed biofilm-membrane bioreactor under a continuous-flowing mode.

This investigation demonstrated that aerobic granular sludge (AGS) could be cultivated rapidly in a single continuous-flowing membrane bioreactor (MBR) by introducing freely moved bio-carriers with a filling ratio of 10%. By operating the bioreactor for 28 days, AGS was successfully cultivated and kept stable for >2 months with a compact structure and clear shape, in which, extracellular polymeric substances played a key role in maintaining the stability of granular sludge structure. The microbial composition between AGS and attached biofilm was quite different, which indicated that the introduced bio-carriers improved the biodiversity within the bioreactor. Additionally, an explicit internal circulation was formed by the introduced bio-carriers, which was the main reason leading to the rapid formation of AGS. This is an interesting discovery and a novel approach to promote the rapid granulation of biomass in an MBR. Moreover, combining the biodegradation of AGS and filtration of membrane module, the bio-reactor achieved an excellent performance in removing CODCr (>90%) and TN (>85%) during the whole process.

Build-up of a continuous flow pre-coated dynamic membrane filter to treat diluted textile wastewater and identify its dynamic membrane fouling.

This research built up a continuous dynamic flow filter membrane to treat diluted textile wastewater and basically investigated dynamic membrane fouling mechanism. By pre-depositing particles activated carbon (PAC) on membrane support material (MSM), a thin layer was formed on its surface, which showed excellent results in removing organic pollutants from diluted textile wastewater. Experimental data were regressed by the Langmuir, Freundlich, Temkin, Dubinin-Radushkevich (D-R) and Sips isotherm models. The three two-parameter isotherms (Temkin, D-R and Freundlich) were the models that best fitted, with respectively 0.977, 0.975 and 0.973 regression coefficients. D-R model has registered the maximum calculated adsorption capacity Qmd, cal. = 45.499 mg/g and the mean energy which was required to adsorb 1 mol of MB dye by the DM layer E = 4.249 kJ/mol; indicating the energy distribution onto heterogeneous surface of a physical adsorption process. Furthermore, kinetic models results showed that MB adsorption onto PAC at different initial concentrations follows the pseudo-second order. The obtained results also indicated that a flexible DM layer with different thickness can be formed from different amount of PAC pre-deposited on MSMs, which demonstrated that it was convenient to adjust the required DM thickness to filtrate a known initial concentration for >99% organic pollutants removal efficiency rate. However, DM fouling occurred on small pores MSMs; which resulted in an increase of the filtration pressure what have affected the filtration performance. PAC and MSMs surface morphology and texture structure, before and after filtration, were visualized respectively by Field Emission Scanning Electron Microscopy (FESEM), Fourier Transform Infra-Red and Attenuated Total Reflectance (FTIR/ATR). From these experimental results, a sustainable flux (>6.85 × 10-5 m/s) was established to discriminate no fouling from fouling conditions based on flux and TMP trends variance.

Residual micro organic pollutants and their biotoxicity of the effluent from the typical textile wastewater treatment plants at Pearl River Delta.

This work investigated the biotoxicity and the residual dissolved organic matter (DOM) of the effluents from nine typical full-scale textile plants located at Pearl River Delta (PRD) in Guangdong province, China. The fluorescence regional integration (FRI) analysis showed that the tryptophan-like (II), soluble microbial product-like (IV) and fulvic acid-like substances (III) were the dominant compounds in the DOM. The acute toxicity test showed toxic effects still remained in most textile effluents, which might attribute to the undegraded dyes or aromatic compounds. Combining with the results from multiple methods, it indicated that the selected nine textile wastewater treatment plants (tWWTPs) all contained some residual micro organic pollutants in their effluents, and the residual benzene-derived products or aromatic amines were probably the toxicity-causing substances. Both ozonization and membrane filtration were capable of further decreasing the content of residual DOM, but by comprehensively considering the effects of removing DOM and biotoxicity, membrane filtration was better than ozonization.

Rapid reformation of larger aerobic granular sludge in an internal-circulation membrane bioreactor after long-term operation: Effect of short-time aeration.

The investigation aimed at revealing the influence of an external disturbance on the rapid reformation of larger aerobic granular sludge (AGS) in an internal-circulation membrane bioreactor (IC-MBR) after long-term operation. The used IC-MBR was continuously operated well for more than one year, in which, the biomass was still in the state of AGS with a balanced average size at around 200 µm and an even size distribution. By providing short-time aeration to the biomass within this bioreactor, the characteristics of biomass were totally changed in a very short time, including the surface hydrophilicity, physic-chemical properties, and the structure of microbial community, which created suitable conditions for the growth of filamentous bacteria (Saccharibacteria). Such a variation was very beneficial to the reformation of larger AGS, which resulted in the average size of AGS increased to nearly 400 µm with a compact structure and clear edge in no more than one month.

Heterogeneity of the diverse aerobic sludge granules self-cultivated in a membrane bioreactor with enhanced internal circulation.

The present work revealed the heterogeneity of the sludge granules formed in a membrane bioreactor with enhanced internal circulation, and also contributed to better understanding of their forming mechanisms. By continuously carrying out an experiment lasting for more than 3 months with the floc sludge from a local municipal wastewater treatment plant as inoculation sludge, diverse aerobic sludge granules were found to be successfully self-cultivated within the reactor. The results of scanning electron microscopy, fluorescence microscope and high-throughput sequencing measurement indicated that the obtained diverse granules exhibited quite obvious heterogeneity in their basic physico-chemical and microbial properties, and filamentous bacteria actually acted as a main skeleton to keep the self-cultivated sludge granules stable in both their structure and morphology. Furthermore, stable and high COD and TN removal achieved, over 85% and 60%, respectively, which confirmed its usefulness in wastewater treatment.

Insight into the microbial community and its succession of a coupling anaerobic-aerobic biofilm on semi-suspended bio-carriers.

This work aims at establishing a coupling anaerobic-aerobic biofilm within a single bioreactor and revealing its microbial community and succession. By using a semi-suspended bio-carrier fabricated with 3D printing technique, an obvious DO gradient was gradually created within the biofilm, which demonstrated that a coupling anaerobic-aerobic biofilm was successfully established on the surface of bio-carriers. The results of metagenomic analysis revealed that the microbial community on the bio-carriers experienced a continuous succession in its structure and dominant species along with the operational time. The formed coupling biofilm created suitable micro multi-habitats for the co-existence of these microorganisms, including nitrifying and denitrifying bacteria, which were beneficial to the removing of organic pollutants and converting nutrients. Along with the succession, the microbial community was gradually dominated by several functional microorganisms. Overall, the results presented an approach to improve the microbial biodiversity by constructing a new structure and floating status of bio-carriers.

Variation of the characteristics of biofilm on the semi-suspended bio-carrier produced by a 3D printing technique: Investigation of a whole growing cycle.

The presented investigation focused on exploring the characteristics of the biofilm formed on a novel semi-suspended bio-carrier and revealing their variation during the whole growing cycle. This used semi-suspended bio-carrier was designed to be a spindle shape, and then fabricated by using a 3D printing technique. Results indicated the bio-carrier provided a suitable environment for the attachment of diverse microorganisms. During the experimental period lasted for 45days, the biofilm quickly attached on the surface of the bio-carrier and grew to maturity, but its characteristics, including the chemical compositions, adhesion force, surface roughness, structure of microbial communities, varied continuously along with the operational time, which greatly influenced the performance of the bioreactor. The shape and structure of bio-carrier, and the shearing force caused by the aeration are important factors that influence the microbial community and its structure, and also heavily affect the formation and growth of biofilm.

Determination of the profile of DO and its mass transferring coefficient in a biofilm reactor packed with semi-suspended bio-carriers.

The work aims at illustrating the profile of DO and its mass transferring process in a biofilm reactor packed with a novel semi-suspended bio-carrier, and further revealing the main factors that influence the mass transferring coefficient of DO within the biofilm. Results showed that the biofilm was very easy to attach and grow on the semi-suspended bio-carrier, which obviously changed the DO profile inside and outside the biofilm. The semi-suspended bio-carrier caused three different mass transfer zones occurring in the bioreactor, including the zones of bulk solution, boundary layer and biofilm, in which, the boundary layer zone had an obvious higher mass transfer resistance. Increasing the aeration rate might improve the hydrodynamic conditions in the bioreactor and accelerate the mass transfer of DO, but it also detached the biofilm from the surface of bio-carrier, which reduced the consumption of DO, and accordingly, decreased the DO gradient in the bioreactor.

Essential factors of an integrated moving bed biofilm reactor-membrane bioreactor: Adhesion characteristics and microbial community of the biofilm.

This work aims at revealing the adhesion characteristics and microbial community of the biofilm in an integrated moving bed biofilm reactor-membrane bioreactor, and further evaluating their variations over time. With multiple methods, the adhesion characteristics and microbial community of the biofilm on the carriers were comprehensively illuminated, which showed their dynamic variation along with the operational time. Results indicated that: (1) the roughness of biofilm on the carriers increased very quickly to a maximum value at the start-up stage, then, decreased to become a flat curve, which indicated a layer of smooth biofilm formed on the surface; (2) the tightly-bound protein and polysaccharide was the most important factor influencing the stability of biofilm; (3) the development of biofilm could be divided into three stages, and Gammaproteobacteria were the most dominant microbial species in class level at the last stage, which occupied the largest ratio (51.48%) among all microbes.