Fenton cleaning strategy for ceramic membrane fouling in wastewater treatment.

Membrane fouling is an obstacle impeding the wide applications of ceramic membranes and organics are responsible for most of the membrane fouling issues in wastewater treatment. In this study, Fenton cleaning strategy was firstly proposed to clean ceramic membrane fouling in wastewater treatment. Fe2+ efficiently catalyzed fouling cleaning with H2O2 (1.5%) to recover the filterability of ceramic membrane. The maximum ∆TMP recovery (over 99%) was achieved at an optimal Fe2+ dosage of 124 mg/L after 6 hr of immersion cleaning. The total residual membrane fouling resistance decreased gradually from this optimum value as the Fe2+ dosage increased above 124 mg/L. The residual hydraulically reversible fouling resistance accounted for most of the membrane fouling and was basically removed (≤3.0 × 109 m-1) when Fe2+ dosages higher than 124 mg/L were used. The foulants responsible for the formation of a residual hydraulically reversible fouling layer (DOC (dissolved organic carbon), proteins, polysaccharides, EEM (fluorescence excitation-emission matrix spectra), SS (suspended solids), and VSS (volatile suspended solids)) were gradually removed as the Fe2+ dosage increased. These residual organic foulants were degraded from biopolymers (10-200 kDa) to low molecular weight substances (0.1-1 kDa), and the particle size of these residual foulants decreased significantly as a result. The strong oxidation power of hydrogen peroxide/hydroxy radicals towards organic foulants was enhanced by Fe2+. Fe2+ played a significant role in the removal of hydraulically reversible fouling and irreversible fouling from the ceramic membrane. However, Fe2+ (≥124 mg/L) increased the likelihood of forming secondary iron-organics aggregates.

Impact of polymeric membrane breakage on drinking water quality and an online detection method of the breakage.

Polymeric membrane has been widely used for the treatment of drinking water in China, and the total treating capacity has reached up to 3.8 million m3/d. However, the membrane breakage found in the membrane modules in many water treatment plants resulted in an increase in turbidity and bacterial amount in the membrane permeate. In this study, a membrane module running for 3 years in a full-scale application was examined in terms of the breaking positions and the numbers of the broken fibers. It was found that most of the breaking positions were mainly on the outlet side of the module and that the distance from these points to the outlet was about 1/10-2/10 length of the membrane module. The lab-scale tests showed that the increase of the numbers of the breaking fibers in the membrane module (the breaking fibers were from 1 to 4 of 75 fibers) resulted in the increase in turbidity, particle count and the amount of total bacteria and coliform bacteria. Meanwhile, the water quality after the filtration with broken membrane fibers was similar to the quality of the raw water, which indicated that once the membrane fiber breakage occurred in the membrane module, the quality of drinking water after membrane filtration was significantly affected. Furthermore, the breaking position closer to the outlet side of the membrane module exposed much higher microbiological risk than those in the middle or near the bottom side. A pilot scale test was conducted by using a membrane module with 6600 fibers, and the effect of the membrane breakage (1-4 broken fibers) on water quality was also investigated. The results indicated that periodical backwashing caused drastic fluctuation of turbidity, particle count and the bacterial amount in the permeate water, which might be due to the washing force and self-blocking action inside the hollow fibers. Moreover, there is a good quantitative relationship (R2 = 0.945) between particle count and the bacterial amount, which indicated that an online detection of particle count can be used to evaluate the bacterial risk. It was also suggested that the online detection of particle count after backwashing within 100 s would be a quick and precise method to identify any fiber breakage in time. These results are very important for the safety issue in the application of polymeric membrane to water treatment plants.

Functionalization of seawater reverse osmosis membrane with quorum sensing inhibitor to regulate microbial community and mitigate membrane biofouling.

Membrane biofouling is a challenge to be solved for the stable operation of the seawater reverse osmosis (SWRO) membrane. This study explored the regulation mechanism of quorum sensing (QS) inhibition on microbial community composition and population-level behaviors in seawater desalination membrane biofouling. A novel antibiofouling SWRO membrane (MA_m) by incorporating one of quorum sensing inhibitors (QSIs), methyl anthranilate (MA) was prepared. It exhibited enhanced anti-biofouling performance than the exogenous addition of QSIs, showing long-term stability and alleviating 22 % decrease in membrane flux compared with the virgin membrane. The results observed that dominant bacteria Epsilon- and Gamma-proteobacteria (Shewanella, Olleya, Colwellia, and Arcobacter), which are significantly related to (P ≤ 0.01) the metabolic products (i.e., polysaccharides, proteins and eDNA), are reduced by over 80 % on the MA_m membrane. Additionally, the introduction of MA has a more significant impact on the QS signal-sensing pathway through binding to the active site of the transmembrane sensor receptor. It effectively reduces the abundance of genes encoding QS and extracellular polymeric substance (EPS) (exopolysaccharides (i.e., galE and nagB) and amino acids (i.e., ilvE, metH, phhA, and serB)) by up to 50 % and 30 %, respectively, resulting in a reduction of EPS by more than 50 %, thereby limiting the biofilm formation on the QSI-modified membrane. This study provides novel insights into the potential of QSIs to control consortial biofilm formation in practical SWRO applications.

Regeneration and utilization of graphite from the spent lithium-ion batteries by modified low-temperature sulfuric acid roasting.

Recycling spent graphite in spent lithium-ion batteries (LIBs) is crucial for lacking high-quality graphite and environmental protection. Here, an environmentally friendly and economical modified method based on sulfate roasting was proposed to recycle spent graphite via low temperature roasting at 250 °C with sodium fluoride as an assistant additive. Recycling leads to graphite with a high purity of 99.55 % and chemical structures for energy storage. Batteries manufactured in regenerated graphite deliver a high initial charge capacity of 333.9 mAh/g with an initial columbic efficiency of 85.71% and excellent capacity retention of 91.2% after 400 cycles. In addition, the waste produced in the method could be well treated, and by-products 177 g of sodium sulfate would be collected per 1 kg spent graphite and NaF, equivalent to 78.95% of the added amount obtained through wastewater and exhaust gas, respectively. The regenerated sodium fluoride will be re-applied to the recovery spent graphite. The loop-closed method shows great promise for the industrial-scale recycling of spent graphite for energy storage applications.

Elucidating the impacts of intermittent in-situ ozonation in a ceramic membrane bioreactor: Micropollutant removal, microbial community evolution and fouling mechanisms.

In this study, impacts of in-situ ozonation applied directly in the membrane tank of a ceramic MBR (Oz-MBR) were assessed to elucidate its implications on micropollutant removal, microbial taxa and membrane fouling. The basic effluent quality (i.e., bulk organics and nutrients) of the MBR without and with in-situ ozonation was comparable. Importantly, pollutant-specific (10-26%) improvement in micropollutant removal was achieved by the Oz-MBR, which could be attributed to the increase in the abundance of microbial taxa responsible for the removal of structurally complex pollutants and/or ozone-assisted oxidation. In-situ ozonation affected the abundance of denitrifying bacteria and functional genes but total nitrogen removal by the Oz-MBR was comparable to that achieved by the control (C)-MBR. Improved mixed liquor properties, and the reduced accumulation of foulants on the membrane surface resulted in membrane fouling alleviation (53%) in the Oz-MBR. In addition, fouling models evaluated for the first time in the case of Oz-MBR indicated that the cake-complete model was suitable to explain membrane fouling mechanism. This comprehensive study demonstrates the performance of MBR coupled with in-situ ozonation, and the obtained results would serve as a useful reference for its implementation at pilot- and/or full-scale.

Electrochemical membrane bioreactors: State-of-the-art and future prospects.

Integration of an electrochemical process with membrane bioreactor (MBR) has attracted considerable attention in the last decade for simultaneous improvement in pollutant removal and hydraulic performance of MBR. Electrochemical MBR (eMBR) with sacrificial anodes has been observed to achieve enhanced phosphorus (up to 40%) and micropollutant removal (5-60%). This is because direct anodic oxidation, indirect oxidation by reactive oxygen species and electrocoagulation can supplement the biological process. The application of an electric field can substantially reduce membrane fouling by 10% to 95% in the eMBR as compared to the conventional MBR. Sacrificial electrodes (e.g., iron or aluminium) have been reported to be more suitable for fouling mitigation than non-sacrificial electrodes (e.g., titanium). However, during prolonged operation, metal ions released from sacrificial electrodes can adversely affect microbial activity and could accumulate in activated sludge. Depending on the current density and electrode material (sacrificial or non- sacrificial), anodic oxidation, electrocoagulation, electrophoresis and/or electroosmosis mechanisms are responsible for suppressing membrane fouling propensity. This paper critically reviews the current status of the electrochemical MBR technology and presents a concise summary of eMBR configurations and electrode materials. Comparative removal of bulk organics, nutrients and micropollutants in the eMBR and conventional MBR is discussed, and performance governing factors are elucidated. Impacts of operating conditions such as current density on mixed liquor properties (e.g., floc size and zeta potential) and microbial activity are elucidated. The extent of membrane fouling mitigation along with associated mechanisms as well as energy consumption is explained and critically analysed. Future research directions are suggested to fast track the scalability of eMBR, which include but are not limited to electrode lifetime, development of self-cleaning conductive membranes, optimisation of operating parameters, removal of emerging micropollutants, accumulation of toxic metals in activated sludge, and degradation by-products and ecotoxicity.

Powdered activated carbon - Membrane bioreactor (PAC-MBR): Impacts of high PAC concentration on micropollutant removal and microbial communities.

In this study, the effect of a high concentration of powdered activated carbon (PAC) on pollutant removal and microbial communities was systematically investigated. Micropollutant removal by the 'control' MBR (without PAC addition) was pollutant-specific and was mainly controlled by their molecular properties. The PAC-MBR achieved enhanced removal of micropollutant by 10% (ofloxacin) to 40% (caffeine). Analysis of the microbial communities in the sludge samples collected from both MBRs indicated an increase in the abundance of 24 (out of 31) genera following PAC addition. Notably, bacterial diversity enriched, particularly in the anoxic zone of the PAC-MBR, indicating a positive impact of recirculating mixed liquor containing PAC from the aerobic to the anoxic zone. In addition, PAC improved the abundance of Comamonas and Methanomethylovorans (up to 2.5%) that can degrade recalcitrant micropollutants. According to the quantitative PCR (qPCR) analysis, the copies of functional genes (nirS, nosZ and narG) increased in PAC-MBR. This study demonstrated that MBR could be operated at a high PAC concentration without compromising the pollutant removal and microbial community evolution during wastewater treatment.

Synergistic effects of combining ozonation, ceramic membrane filtration and biologically active carbon filtration for wastewater reclamation.

In this study, we proposed to apply an integrated process which is comprised of in situ ozonation, ceramic membrane filtration (CMF) and biologically active carbon (BAC) filtration to wastewater reclamation for indirect potable reuse purpose. A pilot-scale (20 m3/d) experiment had been run for ten months to validate the prospect of the process in terms of treatment performance and operational stability. Results showed that the in situ O3 + CMF + BAC process performed well in pollutant removal, with chemical oxygen demand, ammonia, nitrate nitrogen, total phosphorus and turbidity levels in the treated water being 5.1 ±â€¯0.9, 0.05 ±â€¯0.01, 10.5 ±â€¯0.8, <0.06 mg/L, and <0.10 NTU, respectively. Most detected trace organic compounds were degraded by>96%. This study demonstrated that synergistic effects existed in the in situ O3 + CMF + BAC process. Compared to pre-ozonation, in situ ozonation in the membrane tank was more effective in controlling membrane fouling (maintaining operational stability) and in degrading organic pollutants, which could be attributed to the higher residual ozone concentration in the tank. Because of the removal of particulate matter by CMF, water head loss of the BAC filter increased slowly and prolonged the backwashing interval to 30 days. BAC filtration was also effective in removing ammonia and N-nitrosodimethylamine from the ozonated water.

Comparison of long-term ceramic membrane bioreactors without and with in-situ ozonation in wastewater treatment: Membrane fouling, effluent quality and microbial community.

The comparison of long-term ceramic membrane bioreactors (MBRs) without and with in-situ ozonation was investigated in this study in terms of membrane fouling, activated sludge, effluent quality and microbial community in wastewater treatment. The optimal dosage of in-situ ozonation for long-term MBR operation was firstly determined as 5 mg/L (0.66 mg-ozone/g-mixed liquor suspended solid (MLSS)) with the optimal filterability of mixed liquor. During the long-term filtration experiment, MBR-ozone with in-situ ozonation demonstrated its significantly alleviated ceramic membrane fouling performance compared with MBR-control without in-situ ozonation as a result of the enhanced filterability of mixed liquor and organic foulants removal from membrane surface by in-situ ozonation oxidation. Furthermore, ozonation was beneficial to phosphorus removal and the total phosphorus (TP) concentration in effluent of MBR-control (0.82 ±â€¯0.63 mg/L) was >2-fold higher than that of MBR-ozone (0.29 ±â€¯0.41 mg/L). The improved phosphorus removal performance by ozonation was due to the increased abundance of phosphate accumulating bacteria of Candidatus Accumulibacter in activated sludge. However, ozonation was detrimental to nitrogen removal mainly as a result of the inhibition of denitrification with the decreased relative abundance of denitrification genus of Dechloromonas in activated sludge. Overall, ceramic MBR with in-situ ozonation had not only significantly alleviated membrane fouling but also remarkably improved phosphorus removal performance.

Fe(II)-dosed ceramic membrane bioreactor for wastewater treatment: Nutrient removal, microbial community and membrane fouling analysis.

Ferrous dosing is used to reduce phosphorus concentration and alleviate polymeric membrane fouling in membrane bioreactor (MBR). However, limited studies have been conducted to investigate the impacts of ferrous dosing on ceramic membrane fouling, nutrient removal efficiency and microbial community. Accordingly, the aim of this study was to investigate the effect of intermittent ferrous dosing with Fe/P molar ratios of 2 and 1 (with a dosing frequency of every two days) on the overall nutrient removal, functional microbial changes and membrane fouling in ceramic membrane bioreactors (CMBR) in treatment of wastewater. TP concentration of 10 mg/L in influent decreased to 1.94 ±â€¯0.62 mg/L (control), 0.38 ±â€¯0.22 mg/L (Fe/P = 1) and 0.31 ±â€¯0.18 mg/L (Fe/P = 2) in the effluent, respectively. Meanwhile, the effluent total nitrogen (TN) concentrations with Fe/P = 1 treatment (6.80 ±â€¯2.02 mg/L) and Fe/P = 2 treatment (5.12 ±â€¯2.28 mg/L) were lower than that of the control (7.72 ±â€¯2.36 mg/L). Compared to Fe/P = 1, the TN removal performance was better for Fe/P = 2 mainly due to the increased abundance of denitrifying bacteria (Zoogloea and Acinetobacter). In addition, excess iron dose might have toxic effects on bacterial physiology, however the Fe concentrations that cause cell damage vary for different bacteria. The relative abundance of Zoogloea (aerobic denitrifying bacteria) continuously increased with ferrous addition (Fe/P = 2), while other bacteria including Dechloromonas, Hyphomicrobium and Thauera (anoxic denitrifying bacteria), Nitrospira (nitrifying bacteria) and Candidatus Accumulibacter (phosphorus accumulating organism) decreased sharply. Furthermore, membrane fouling was effectively moderated by ferrous dosing and Fe/P = 1 treatment showed improved membrane fouling mitigation than Fe/P = 2. Overall, intermittent ferrous addition in CMBR with Fe/P molar ratio of 1 was beneficial to the removal of nutrients (TP, TN and organics), enhanced succession of microbial community and membrane fouling mitigation.

Effect of ferric and ferrous iron addition on phosphorus removal and fouling in submerged membrane bioreactors.

The effect of continuously dosing membrane bioreactors (MBRs) with ferric chloride (Fe(III)) and ferrous sulphate (Fe(II)) on phosphorus (P) removal and membrane fouling is investigated here. Influent phosphorus concentrations of 10 mg/L were consistently reduced to effluent concentrations of less than 0.02 mg/L and 0.03-0.04 mg/L when an Fe(III)/P molar ratio of 4.0 and Fe/P molar ratio (for both Fe(II) and Fe(III)) of 2.0 were used, respectively. In comparison, effluent concentrations did not decrease below 1.35 mg/L in a control reactor to which iron was not added. The concentrations of supernatant organic compounds, particularly polysaccharides, were reduced significantly by iron addition. The sub-critical fouling time (tcrit) after which fouling becomes much more severe was substantially shorter with Fe(III) dosing (672 h) than with Fe(II) dosing (1200-1260 h) at Fe/P molar ratios of 2.0 while the control reactor (no iron dosing) exhibited a tcrit of 960 h. Not surprisingly, membrane fouling was substantially more severe at Fe/P ratios of 4. Fe(II) doses yielding Fe/P molar ratios of 2 or less with dosing to the aerobic chamber were found to be optimal in terms of P removal and fouling mitigation performance. In long term operation, however, the use of iron for maintaining appropriately low effluent P concentrations results in more severe irreversible fouling necessitating the application of an effective membrane cleaning regime.