Yoshimasa Watanabe

Microfiltration of different surface waters with/without coagulation: clear correlations between membrane fouling and hydrophilic biopolymers.

Although low-pressure membranes (microfiltration (MF) or ultrafiltration (UF)) have become viable options for drinking water treatment, problems caused by membrane fouling must still be addressed. The objective of this study was to compare five different surface waters and to identify a relevant index of water quality that can be used for prediction of the fouling potential of the water. Bench-scale filtration tests were carried out with commercially available hollow-fiber MF membranes. Fairly long-term (a few days) filtrations in the constant-flow mode were carried out with automatic backwash. Membrane fouling in this study was shown to be irreversible as a result of the periodic backwash carried out throughout of the operation. Easily accessible indexes of water quality including dissolved organic carbon (DOC), UV absorbance, Ca concentration and turbidity could not explain the degree of fouling encountered in the filtration tests. Fluorescence excitation-emission matrix (EEM) could provide information on the presence of protein-like substances in water, and peaks for protein showed some correlation with the membrane fouling. Biopolymer (characterized by high molecular weights and insensitivity to UV light absorption) concentrations in the five waters determined by liquid chromatography with organic carbon detection (LC-OCD) exhibited an excellent correlation with the fouling rates. Coagulation with polyaluminum chloride could mitigate membrane fouling in all cases. The extent of fouling seen with coagulated waters was also correlated with biopolymer concentrations. The relationship between biopolymer concentrations and the fouling rates established for the raw waters could also be applied to the coagulated waters. These results suggested that the contribution of biopolymers to membrane fouling in the present study was significant, an observation that was supported by the analysis of foulants extracted at the termination of each test. Biopolymer concentrations determined by LC-OCD might be used as a key indicator of fouling potential of water for low-pressure membranes.

Hydrophilic fraction of natural organic matter causing irreversible fouling of microfiltration and ultrafiltration membranes.

Although membrane filtration is a promising technology in the field of drinking water treatment, persistent membrane fouling remains a major disadvantage. For more efficient operation, causative agents of membrane fouling need to be identified. Membrane fouling can be classified into physically reversible and irreversible fouling on basis of the removability of the foulants by physical cleaning. Four types of natural organic matter (NOM) in river water used as a source of drinking water were fractionated into hydrophobic and hydrophilic fractions, and their potential to develop irreversible membrane fouling was evaluated by a bench-scale filtration experiment together with spectroscopic and chromatographic analyses. In this study, only dissolved NOM was investigated without consideration of interactions of NOM fractions with particulate matter. Results demonstrated that despite identical total organic carbon (TOC), fouling development trends were significantly different between hydrophilic and hydrophobic fractions. The hydrophobic fractions did not increase membrane resistance, while the hydrophilic fractions caused severe loss of membrane permeability. These results were identical with the case when the calcium was added to hydrophobic and hydrophilic fractions. The largest difference in NOM characteristics between hydrophobic and hydrophilic fractions was the presence or absence of macromolecules; the primary constituent causing irreversible fouling was inferred to be biopolymers, including carbohydrates and proteins. In addition, the results demonstrated that the extent of irreversible fouling was considerably different depending on the combination of membrane materials and NOM characteristics. Despite identical nominal pore size (0.1xa0μm), a polyvinylidene fluoride (PVDF) membrane was found to be more rapidly fouled than a PE membrane. This is probably explained by the generation of strong hydrogen bonding between hydroxyl groups of biopolymers and fluorine of the PVDF membrane. On the basis of these findings, it was suggested that the higher fouling potential of the hydrophilic fraction of the dissolved NOMs from various natural water sources are mainly attributed to macromolecules, or biopolymers.

High efficiency removal of phosphate from water by zirconium sulfate-surfactant micelle mesostructure immobilized on polymer matrix

A zirconium sulfate-surfactant micelle mesostructure (ZS) was synthesized to investigate its capacity for phosphate removal from water. Its phosphate adsorption kinetics, the effect of pH and interfering anions, adsorption isotherm, desorption capacity, and reusability were investigated. The adsorption isotherms could be described by the Langmuir model. The ZS was an effective adsorbent for phosphate with a very high adsorption capacity (114 mg P/g ZS). The phosphate adsorption capacity increased with decrease in pH. Although the adsorption of nitrate, chloride and acetate ions was negligible, bicarbonate ions were found to be possible interfering anions. The adsorbed phosphate was desorbed effectively using NaOH solution. Since breakage of ZS particles resulted when using NaOH, ZS was immobilized on a polymer matrix and a 50-cycle adsorption-desorption test was carried out to determine the ZS-immobilized polymer (P-ZS) reusability. The P-ZS retained its functionality and adsorption and desorption capacity over 50 cycles without loss of original capacity. A phosphate solution containing about 10 mg P/L was treated in a column packed with P-ZS. The phosphate could be adsorbed completely onto P-ZS up to 1020 bed volumes. These results indicate clearly that ZS is a highly effective adsorbent for phosphate and enables the removal of phosphate from water.

Influence of extracellular polysaccharides (EPS) produced by two different green unicellular algae on membrane filtration in an algae-based biofuel production process

In the present study, two strains of green algae named S1 and S2, categorized as the same species of Pseudo-coccomyxa ellipsoidea but showing 99% homology, were cultivated under the same conditions and filtrated with a microfiltration membrane. On the basis of the results of the extracellular polysaccharides (EPS) characteristics of these two green algae and the degree of fouling, the influence of these characteristics on the performance of membrane filtration was investigated. There was no difference in the specific growth rate between the S1 and S2 strains; however, large differences were seen in the amount and quality of EPS between S1 and S2. When the S1 and S2 strains were filtered with a membrane, the trend in the increase in transmembrane pressure (TMP) was quite different. The filtration of the S1 strain showed a rapid increase in TMP, whereas the TMP of the filtration of the S2 strain did not increase at all during the operation. This clearly demonstrated that the characteristics of each strain affect the development of membrane fouling. On the basis of the detailed characterization of solved-EPS (s-EPS) and bound-EPS (b-EPS), it was clarified that s-EPS mainly contributed to irreversible fouling for both operations and the biopolymer-like organic matter contained in b-EPS mainly contributed to reversible fouling.

Flocculation and me

This paper is mainly a review of the authors previous research, which was aimed at establishing a theoretical protocol for the design and operation of flocculators based on data from experiments and simulations of the flocculation process. Flocculation is the main pretreatment process of the rapid sand filtration system, and the process produces settleable flocs in the sedimentation basin, reducing the solid load flowing to the sand filter. We tried to make the transition from empirical to theoretical approaches in the design and operation of flocculators by combining the three categories of flocculation research: floc characteristics, flocculation kinetics, and engineering aspects of flocculation. The floc density function and the floc strength function were proposed as important attributes of floc. The Levichs Equation, based on the assumption of viscous subrange diffusion control, represented the basic collision kinetics during flocculation. Finally, examples of engineering applications using our flocculation research were described.

Performance of anaerobic membrane bioreactor during digestion and thickening of aerobic membrane bioreactor excess sludge

In this study, we evaluated the performance of an anaerobic membrane bioreactor in terms of digestion and thickening of excess sludge from an aerobic membrane bioreactor. A digestion reactor equipped with an external polytetrafluoroethylene tubular microfiltration membrane module was operated in semi-batch mode. Solids were concentrated by repeated membrane filtration and sludge feeding, and their concentration reached 25,400mg/L after 92d. A high chemical oxygen demand (COD) removal efficiency, i.e., 98%, was achieved during operation. A hydraulic retention time of 34d and a pulse organic loading rate of 2200mg-COD/(L-reactor) gave a biogas production rate and biogas yield of 1.33L/(reactor d) and 0.08L/g-CODinput, respectively. The external membrane unit worked well without membrane cleaning for 90d. The transmembrane pressure reached 25kPa and the filtration flux decreased by 80% because of membrane fouling after operation for 90d.

Changes in the physical properties of the dynamic layer and its correlation with permeate quality in a self-forming dynamic membrane bioreactor

The self-forming dynamic membrane bioreactor (SFDMBR) is a biological wastewater treatment technology based on the conventional membrane bioreactor (MBR) with membrane material modification to a large pore size (30-100u202fμm). This modification requires a dynamic layer formed by activated sludge to provide effective filtration function for high-quality permeate production. The properties of the dynamic layer are therefore important for permeate quality in SFDMBRs. The interaction between the structure of the dynamic layer and the performance of SFDMBRs is little known but understandably complex. To elucidate the interaction, a lab-scale SFDMBR system coupled with a nylon woven mesh as the supporting material was operated. After development of a mature dynamic layer, excellent solid-liquid separation was achieved, as evidenced by a low permeate turbidity of less than 2 NTU. The permeate turbidity stayed below this level for nearly 80 days. In the fouling phase, the dynamic layer was compressed with an increase in the trans-membrane pressure and the quality of the permeate kept deteriorating until the turbidity exceeded 10 NTU. The investigation revealed that the majority of permeate particles were dissociated from the dynamic layer on the back surface of the supporting material, which is caused by the compression, breakdown, and dissociation of the dynamic layer. This phenomenon was observed directly in experiment instead of model prediction or conjecture for the first time.

Development of novel polysulfone membranes with embedded zirconium sulfate-surfactant micelle mesostructure for phosphate recovery from water through membrane filtration

We prepared novel membranes that could adsorb phosphate from water through membrane filtration for use in a phosphate recovery system. Zirconium sulfate surfactant micelle mesostructure (ZS), which was the phosphate adsorbent, was embedded in a polysulfone matrix and flat sheet ultrafiltration membranes were made by nonsolvent induced phase separation. Scanning electron microscopy showed that the ZS particles existed on both the top surface and in the internal surface of the membrane. Increases in ZS content led to greater pure water flux because of increases in the surface porosity ratio. The amount of phosphate adsorbed on the membrane made from the polymer solution containing 10.5xa0wt% ZS was 0.071xa0mgxa0P/cm2 (64.8xa0mgxa0P/g-ZS) during filtration of 50xa0mgxa0P/L synthetic phosphate solution. The membrane could be repeatedly used for phosphate recovery after regeneration by filtration of 0.1xa0M NaOH solution to desorb the phosphate. We applied the membrane to treat the effluent from an anaerobic membrane bioreactor as a real sample and successfully recovered phosphate.

Proteins causing membrane fouling in membrane bioreactors.

In this study, the details of proteins causing membrane fouling in membrane bioreactors (MBRs) treating real municipal wastewater were investigated. Two separate pilot-scale MBRs were continuously operated under significantly different operating conditions; one MBR was a submerged type whereas the other was a side-stream type. The submerged and side-stream MBRs were operated for 20 and 10 days, respectively. At the end of continuous operation, the foulants were extracted from the fouled membranes. The proteins contained in the extracted foulants were enriched by using the combination of crude concentration with an ultrafiltration membrane and trichloroacetic acid precipitation, and then separated by two-dimensional polyacrylamide gel electrophoresis (2D-PAGE). The N-terminal amino acid sequencing analysis of the proteins which formed intensive spots on the 2D-PAGE gels allowed us to partially identify one protein (OmpA family protein originated from genus Brevundimonas or Riemerella anatipestifer) from the foulant obtained from the submerged MBR, and two proteins (OprD and OprF originated from genus Pseudomonas) from that obtained from the side-stream MBR. Despite the significant difference in operating conditions of the two MBRs, all proteins identified in this study belong to β-barrel protein. These findings strongly suggest the importance of β-barrel proteins in developing membrane fouling in MBRs.

Tracking inorganic foulants irreversibly accumulated on low-pressure membranes for treating surface water

While low-pressure membrane filtration processes (i.e., microfiltration and ultrafiltration) can offer precise filtration than sand filtration, they pose the problem of reduced efficiency due to membrane fouling. Although many studies have examined membrane fouling by organic substances, there is still not enough data available concerning membrane fouling by inorganic substances. The present research investigated changes in the amounts of inorganic components deposited on the surface of membrane filters over time using membrane specimens sampled thirteen times at arbitrary time intervals during pilot testing in order to determine the mechanism by which irreversible fouling by inorganic substances progresses. The experiments showed that the inorganic components that primarily contribute to irreversible fouling vary as filtration continues. It was discovered that, in the initial stage of operation, the main membrane-fouling substance was iron, whereas the primary membrane-fouling substances when operation finished were manganese, calcium, and silica. The amount of iron accumulated on the membrane increased up to the thirtieth day of operation, after which it reached a steady state. After the accumulation of iron became static, subsequent accumulation of manganese was observed. The fact that the removal rates of these inorganic components also increased gradually shows that the size of the exclusion pores of the membrane filter narrows as operation continues. Studying particle size distributions of inorganic components contained in source water revealed that while many iron particles are approximately the same size as membrane pores, the fraction of manganese particles slightly smaller than the pores in diameter was large. From these results, it is surmised that iron particles approximately the same size as the pores block them soon after the start of operation, and as the membrane pores narrow with the development of fouling, they become further blocked by manganese particles approximately the same size as the narrowed pores. Calcium and silica are assumed to accumulate on the membrane due to their cross-linking action and/or complex formation with organic substances such as humic compounds. The present research is the first to clearly show that the inorganic components that contribute to membrane fouling differ according to the stage of membrane fouling progression; the information obtained by this research should enable chemical cleaning or operational control in accordance with the stage of membrane fouling progression.