Haloketones (HKs) is one class of disinfection by-products (DBPs) which is genetically toxic and mutagenic. Monitoring HKs in drinking water is important for drinking water safety, yet it is a ...time-consuming and laborious job. Developing predictive models of HKs to estimate their occurrence in drinking water is a good alternative, but to date no study was available for HKs modeling. This study was to explore the feasibility of linear, log linear regression models, back propagation (BP) as well as radial basis function (RBF) artificial neural networks (ANNs) for predicting HKs occurrence (including dichloropropanone, trichloropropanone and total HKs) in real water supply systems. Results showed that the overall prediction ability of RBF and BP ANNs was better than linear/log linear models. Though the BP ANN showed excellent prediction performance in internal validation (N25 = 98–100%, R2 = 0.99–1.00), it could not well predict HKs occurrence in external validation (N25 = 62–69%, R2 = 0.202–0.848). Prediction ability of RBF ANN in external validation (N25 = 85%, R2 = 0.692–0.909) was quite good, which was comparable to that in internal validation (N25 = 74–88%, R2 = 0.799–0.870). These results demonstrated RBF ANN could well recognized the complex nonlinear relationship between HKs occurrence and the related water quality, and paved a new way for HKs prediction and monitoring in practice.
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•Linear/log linear regression models cannot well predict haloketones (HKs) levels.•Back propagation (BP) is good to predict HKs in internal but bad in external validation.•Radial basis function artificial neural network (RBF ANN) well predicts HKs levels.•RBF ANN can well recognize complex relationships between HKs and water quality.
Though sludge foaming often occurs and thus causes serious membrane fouling in membrane bioreactors (MBRs), the fouling mechanisms related with the foaming phenomenon have not been well addressed, ...hindering better understanding and solving foaming problem. In this work, it was interestingly found that, the foulants during the foaming period possessed extremely high specific filtration resistance (SFR) (over 1016 m kg−1) and strong adhesion ability to membrane surface. Chemical characterization showed that the proteins (178.57 mg/L) and polysaccharides (209.21 mg/L) in the foaming sample were about 6.4 times and 5.4 times of those in the supernatant sample, suggesting existence of a mechanism permitting continuous production of these foulants in the MBR during the foaming period. It was revealed that the fouling caused by foams was associated with gel layer filtration process, and the extremely high SFR can be interpreted by chemical potential change in the gel filtration process depicted in Flory-Huggins theory. Meanwhile, analyses by the extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) theory showed that the strong adhesion ability stemmed from the high interaction energy between the foaming foulants and membrane surface. In addition, 16S rDNA gene sequencing identified that the abundance of the foaming related bacteria species in the sludge suspension during the foaming period was more than 10 times of that during the non-foaming period. This study offered new mechanism insights into foaming fouling in MBRs.
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•Foaming foulants had a high specific filtration resistance (SFR) of 1.11 × 1016 m kg−1•There is a mechanism permitting continuous production of foaming foulants in the MBR.•High foaming SFR was related with gel filtration and caused by chemical potential gap.•The strong adhesion ability of foams stemmed from the high interaction energy.•Abundance of foaming related bacteria is 10 times of that during non-foaming period.
Soluble microbial products (SMPs) are the predominate foulants determining fouling extent in membrane bioreactors (MBRs). However, exact mechanism underlying their typical fouling behaviors remains ...unrevealed. In this study, the typical fouling behaviors of SMPs during initial operational period of a MBR were characterized. It was found that, although being low content, SMPs rather than sludge particulates preferentially adhered to membrane surface to accumulate a gel layer, and moreover, specific filtration resistance (SFR) of SMPs was approximately 700 times larger than that of the sludge particulates at operational day 3. According to energy balance principle, a unified thermodynamic mechanism underlying these fouling behaviors of SMPs was proposed. Thermodynamic analyses demonstrated that, the attractive interaction energy strength in contact between SMPs and membrane was larger by around 3700 times than that between sludge particulates and membrane, well explaining the extremely high adhesive ability of SMPs over sludge particlulates. Meanwhile, filtration through a SMPs layer was modelled and simulated as a thermodynamic process. Simulation on an agar gel showed that, about 92.6% of SFR was originated from mixing free energy change during filtration. Such a result satisfactorily interpreted the extremely high SFR of SMPs layer over sludge cake layer. The revealed thermodynamic mechanism underlying SMPs fouling behaviors significantly deepened understanding of fouling, and facilitated to development of effective fouling control strategies.
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•Soluble microbial products (SMPs) preferentially adhered to membrane surface.•Specific filtration resistance (SFR) of SMPs was about 700 times of sludge SFR.•A unified thermodynamic mechanism of SMPs' fouling behaviors was proposed.•Interaction energy strength for SMPs was about 3700 times of that for sludge particulates.•About 92.6% of SFR was originated from mixing free energy change in SMPs filtration.
In the last years, anaerobic membrane bioreactor (AnMBR) technology is being considered as a very appealing alternative for wastewater treatment due to the significant advantages over conventional ...anaerobic treatment and aerobic membrane bioreactor (MBR) technology. Many articles have touted the diverse potential applications of AnMBR in various stream treatment, and membrane fouling issues. In current review, the fundamentals of AnMBR (including advantages and configurations, membrane materials and modules, and history development), application development in various stream treatment, and membrane fouling researches are summarized and critically assessed. The characteristics of AnMBR and aerobic MBR for wastewater treatment are also compared. AnMBR technology appears to be suitable for treatment of various streams, especially for food industrial wastewater and municipal wastewater. AnMBR treatment usually encounters more serious membrane fouling problem. This, however, can be remedied through various conventional and novel membrane fouling control or cleaning measures. Based on the review, future research perspectives relating to its application and membrane fouling research are proposed.
► Recent progress in AnMBRs treating various wastewaters is summarized. ► Advances in membrane fouling control strategies in AnMBRs are addressed. ► Research directions regarding AnMBR technology are identified. ► AnMBR is a promising technology for wastewater treatment and reuse.
Extracellular polymeric substances (EPSs) are key biological substances, which largely determine properties of sludge flocs, including hydrophobicity, adhesion, flocculation, settling and dewatering ...properties, and therefore significantly affect membrane fouling in membrane bioreactors (MBRs). Much progress has been achieved in understanding of EPSs and their interrelations with membrane fouling due to a large number of systematic papers published in the last three decades. In this paper, the fundamentals of EPSs including definitions, compositions and properties are summarized. The interrelations of EPSs with other foulants in MBRs are clarified. Roles of EPSs in membrane fouling mechanisms in MBRs are critically assessed. Furthermore, factors affecting EPSs production and characteristics are summarized, and based on which, EPSs control towards membrane fouling mitigation in MBRs are comprehensively discussed. Finally, future research perspectives regarding EPSs and membrane fouling are proposed.
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•Fundamentals of EPSs including composition and properties are summarized.•Roles of EPSs in membrane fouling in MBRs are addressed.•Factors affecting EPSs in MBRs are summarized.•Strategies of EPSs control towards fouling mitigation are discussed.•Research directions regarding fouling caused by EPSs are identified.
Fouling behaviors of polysaccharides vary with their structure, while the mechanisms underlying this phenomenon remain unexplored. This work was carried out to explore the thermodynamic fouling ...mechanisms of polysaccharides with different structure. Carrageenan and xanthan gum were selected as the model polysaccharides with structure of straight and branch chains, respectively. Batch filtration experiments showed that xanthan gum solution corresponded to a more rapid flux decline trend, and specific filtration resistance (SFR) of xanthan gum (2.32 × 1015 m−1 kg−1) was over 10 times than that of carrageenan (2.21 × 1014 m−1 kg−1). It was found that, xanthan gum possessed a more disordered structure and a rather higher viscosity (15.03 mPa·s V.S. 1.98 mPa·s for carrageenan). Calculation of extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) theory showed higher adhesion energy of xanthan gum (−42.82 my m−2 V.S. −23.26 mJ m−2 for carrageenan). Scanning electron microscopy (SEM) analyses showed that xanthan gum gel layer had a more homogenous structure and rigid polymer backbone, indicating better mixing with water to form a gel. As verified by heating experiments, such a structure tended to contain more bound water. According to this information, Flory-Huggins lattice theory was introduced to build a bridge between polymeric structure and SFR. It was revealed that branch structure corresponded to higher chemical potential change during gel layer formation, and higher ability to carry bound water, resulting in higher filtration resistance during filtration process. This work revealed the fundamental thermodynamic mechanism of membrane fouling caused by polysaccharides with different structure, deepening understanding of membrane fouling.
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•Specific filtration resistance (SFR) of xanthan gum was about 10 times than that of carrageenan.•Molecular structure contributed to higher adhesion energy of xanthan gum to membrane surface.•Gel formation of xanthan gum corresponded to higher chemical potential change and SFR.•Thermodynamic mechanisms governed polysaccharides' adhesion and gel layer filtration process.
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•Gel layer was more easily formed when SMP content was relatively high.•Gel adhesion had higher contact interaction energy but had repulsive energy barrier.•Gel layer had a SFR which ...was about 100 times higher than that of cake layer.•The unusually high SFR of gel layer was caused by osmotic pressure mechanism.
The fouling mechanisms underlying gel layer formation and its filtration resistance in a submerged membrane bioreactor (MBR) were investigated. It was found that gel layer rather than cake layer was more easily formed when soluble microbial products content in sludge suspension was relatively high. Thermodynamic analyses showed that gel layer formation process should overcome a higher energy barrier as compared with cake layer formation process. However, when separation distance <2.3nm, attractive interaction energy of gelling foulant–membrane combination was remarkably higher than that of sludge floc–membrane combination. The combined effects were responsible for gel layer formation. Filtration tests showed that specific filtration resistance (SFR) of gel layer was almost 100 times higher than that of cake layer. The unusually high SFR of gel layer could be ascribed to the gelling propensity and osmotic pressure mechanism. These findings shed significant light on fouling mechanisms of gel layer in MBRs.
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•SFR variation of alginate complexes with PACl dosage showed a unimodal pattern.•Alginate gel at PACl dosage of 100 mg/L had an ultra-high value of 1.40 × 1015 m−1 kg−1.•Unimodal ...pattern of SFR was caused by morphology transition from gel to floc.•Morphology transition was caused by the coordination order of Al3+with COOH.•Ultra-high gel SFR could be interpreted by Flory–Huggins lattice theory.
While polyaluminum chloride (PACl) coagulation- microfiltration (MF) process is one of the most popular methods for surface water treatment, the fouling mechanism underlying this process has not well explored. In this study, sodium alginate (SA) was used as the model organic matter. It was interestingly found that, specific filtration resistance (SFR) of alginate-aluminum complexes initially increased to an ultra-high value of 1.40 × 1015 m−1 kg−1, and then sharply declined to rather low level of 3.85 × 1012 m−1 kg−1 with the increase in PACl dosage from 0 to 500 mg/L. A series of characterizations of the foulant samples showed that the alginate-aluminum complexes suffered a morphology transition from gel form to floc/cake form with the PACl dosage increase. Density functional theory (DFT) calculation indicated the preferential coordination of aluminum ions with the terminal carboxyl groups of the alginate chains at low PACl level, facilitating homogeneous gel formation. The ultra-high SFR of gel was interpreted by the Flory-Huggins lattice theory. High PACl level resulted in the coordination of aluminum ions with the non-terminal carboxyl groups and reduced the surface charge, and thus, caused gel collapse and floc formation, corresponding to rather low SFR values. Preferential coordination combined with the Flory-Huggins lattice theory revealed in this study offered a molecular level fouling mechanism in the coagulation- microfiltration (MF) process for water treatment.
The interfacial interactions between sludge foulants and four different types of membranes were assessed based on a new combined calculation method. Effects of membrane surface ...hydrophilicity/hydrophobicity on the interfacial interactions were investigated. It was found that, membrane surface hydrophilicity/hydrophobicity was not directly relevant to the interfacial interactions with sludge particles. Increasing membrane surface zeta potential could significantly increase the strength of the electrostatic double layer (EL) interaction and the energy barrier. For membrane with a surface roughness of 300nm, the total interaction was continuously repulsive in the separation distance coverage of 0-4nm in this study. The results suggest that, under conditions in this study, designing membranes with a high zeta potential and certain roughness can significantly mitigate membrane fouling, whereas, the strategy of improving membrane surface hydrophilicity cannot alleviate sludge adhesion in the membrane bioreactor.
The formations of THMs, HAAs, and HNMs from chlorination and chloramination of water from Jinlan Reservoir were investigated in this study. Results showed that monochloramine rather than chlorine ...generally resulted in lower concentration of DBPs, and the DBPs formation varied greatly as the treatment conditions changed. Specifically, the yields of THMs, HAAs and HNMs all increased with the high bromide level and high disinfectant dose both during chlorination and chloramination. The longer reaction time had a positive effect on the formation of THMs, HAAs and HNMs during chlorination and HNMs during chloramination. However, no time effect was observed on the formation of THMs and HAAs during chloramination. An increase in pH enhanced the levels of THMs and HNMs upon chlorination but reduced levels of HNMs upon chloramination. As for the THMs in chloramination and HAAs in chlorination and chloramination, no obvious pH effect was observed. The elevated temperature significantly increased the yields of THMs during chlorination and HNMs during chloramination, but has no effect on THMs and HAAs yields during chloramination. In the same temperature range, the formation of HAAs and HNMs in chlorination showed a first increasing and then a decreasing trend. In chloramination study, addition of nitrite markedly increased the formation of HNMs but had little impact on the formation of THMs and HAAs. While in chlorination study, the presence of high nitrite levels significantly reduced the yields of THMs, HAAs and HNMs. Range analysis revealed that the bromide and disinfectant levels were the major factors affecting THMs, HAAs and HNMs formation, in both chlorination and chloramination. Finally, comparisons of the speciation of mono-halogenated, di-halogenated, tri-halogenated HAAs and HNMs between chlorination and monochloramination were also conducted, and factors influencing the speciation pattern were identified.
► NH2Cl generally produced lower THMs, HAAs and HNMs yields than Cl2. ► Bromide level and disinfectant dose are two most important factors affecting THMs, HAAs and HNMs formation. ► Addition of nitrite significantly increased HNMs formation during chloramination, but was not necessary in the chlorination. ► The factors affect the speciation of mono-halogenated, dihalogenated, and trihalogenated HAAs and HNMs were assessed.
