Role of feed water biodegradable substrate concentration on biofouling: Biofilm characteristics, membrane performance and cleanability.

Biofouling severely impacts operational performance of membrane systems increasing the cost of water production. Understanding the effect of critical parameters of feed water such as biodegradable substrate concentration on the developed biofilm characteristics enables development of more effective biofouling control strategies. In this study, the effect of substrate concentration on the biofilm characteristics was examined using membrane fouling simulators (MFSs). A feed channel pressure drop (PD) increase of 200 mbar was used as a benchmark to study the developed biofilm. The amount and characteristics of the formed biofilm were analysed in relation to membrane performance indicators: feed channel pressure drop and permeate flux. The effect of the characteristics of the biofilm developed at three substrate concentrations on the removal efficiency of the different biofilms was evaluated applying acid/base cleaning. Results showed that a higher feed water substrate concentration caused a higher biomass amount, a faster PD increase, but a lower permeate flux decline. The permeate flux decline was affected by the spatial location and the physical characteristics of the biofilm rather than the total amount of biofilm. The slower growing biofilm developed at the lowest substrate concentration was harder to remove by NaOH/HCl cleanings than the biofilm developed at the higher substrate concentrations. Effective biofilm removal is essential to prevent a fast biofilm regrowth after cleaning. While substrate limitation is a generally accepted biofouling control strategy delaying biofouling, development of advanced cleaning methods to remove biofilms formed under substrate limited conditions is of paramount importance.

Enhanced biofilm solubilization by urea in reverse osmosis membrane systems.

Chemical cleaning is routinely performed in reverse osmosis (RO) plants for the regeneration of RO membranes that suffer from biofouling problems. The potential of urea as a chaotropic agent to enhance the solubilization of biofilm proteins has been reported briefly in the literature. In this paper the efficiency of urea cleaning for RO membrane systems has been compared to conventionally applied acid/alkali treatment. Preliminary assessment confirmed that urea did not damage the RO polyamide membranes and that the membrane cleaning efficiency increased with increasing concentrations of urea and temperature. Accelerated biofilm formation was carried out in membrane fouling simulators which were subsequently cleaned with (i) 0.01M sodium hydroxide (NaOH) and 0.1M hydrochloric acid (HCl) (typically applied in industry), (ii) urea (CO(NH2)2) and hydrochloric acid, or (iii) urea only (1340 g/Lwater). The pressure drop over the flow channel was used to evaluate the efficiency of the applied chemical cleanings. Biomass removal was evaluated by measuring chemical oxygen demand (COD), adenosine triphosphate (ATP), protein, and carbohydrate content from the membrane and spacer surfaces after cleaning. In addition to protein and carbohydrate quantification of the extracellular polymeric substances (EPS), fluorescence excitation-emission matrix (FEEM) spectroscopy was used to distinguish the difference in organic matter of the remaining biomass to assess biofilm solubilization efficacy of the different cleaning agents. Results indicated that two-stage CO(NH2)2/HCl cleaning was as effective as cleaning with NaOH/HCl in terms of restoring the feed channel pressure drop (>70% pressure drop decrease). One-stage cleaning with urea only was not as effective indicating the importance of the second-stage low pH acid cleaning in weakening the biofilm matrix. All three chemical cleaning protocols were equally effective in reducing the concentration of predominant EPS components protein and carbohydrate (>50% reduction in concentrations). However, urea-based cleaning strategies were more effective in solubilizing protein-like matter and tyrosine-containing proteins. Furthermore, ATP measurements showed that biomass inactivation was up to two-fold greater after treatment with urea-based chemical cleanings compared to the conventional acid/alkali treatment. The applicability of urea as an alternative, economical, eco-friendly and effective chemical cleaning agent for the control of biological fouling was successfully demonstrated.

Porosity of spacer-filled channels in spiral-wound membrane systems: Quantification methods and impact on hydraulic characterization.

The porosity of spacer-filled feed channels influences the hydrodynamics of spiral-wound membrane systems and impacts the overall performance of the system. Therefore, an exact measurement and a detailed understanding of the impact of the feed channel porosity is required to understand and improve the hydrodynamics of spiral-wound membrane systems applied for desalination and wastewater reuse. The objectives of this study were to assess the accuracy of porosity measurement techniques for feed spacers differing in geometry and thickness and the consequences of using an inaccurate method on hydrodynamic predictions, which may affect permeate production. Six techniques were applied to measure the porosity namely, three volumetric techniques based on spacer strand count together with a cuboidal (SC), cylindrical (VCC) and ellipsoidal volume calculation (VCE) and three independent techniques based on volume displacement (VD), weight and density (WD) and computed tomography (CT) scanning. The CT method was introduced as an alternative for the other five already existing and applied methods in practice. Six feed spacers used for the porosity measurement differed in filament thickness, angle between the filaments and mesh-size. The results of the studies showed differences between the porosities, measured by the six methods. The results of the microscopic techniques SC, VCC and VCE deviated significantly from measurements by VD, WD and CT, which showed similar porosity values for all spacer types. Depending on the maximum deviation of the porosity measurement techniques from -6% to +6%, (i) the linear velocity deviations were -5.6% and +6.4% respectively and (ii) the pressure drop deviations were -31% and +43% respectively, illustrating the importance of an accurate porosity measurement. Because of the accuracy and standard deviation, the VD and WD method should be applied for the porosity determination of spacer-filled channels, while the CT method is recommended for numerical modelling purposes. The porosity has a linear relationship with the flow velocity and a superlinear effect on the pressure drop. Accurate porosity data are essential to evaluate feed spacer performance in spiral-wound membrane systems. Porosity of spacer-filled feed channels has a strong impact on membrane performance and biofouling impact.

Predicting the impact of feed spacer modification on biofouling by hydraulic characterization and biofouling studies in membrane fouling simulators.

Feed spacers are an essential part of spiral-wound reverse osmosis (RO) and nanofiltration (NF) membrane modules. Geometric modification of feed spacers is a potential option to reduce the impact of biofouling on the performance of membrane systems. The objective of this study was to evaluate the biofouling potential of two commercially available reference feed spacers and four modified feed spacers. The spacers were compared on hydraulic characterization and in biofouling studies with membrane fouling simulators (MFSs). The virgin feed spacer was characterized hydraulically by their resistance, measured in terms of feed channel pressure drop, performed by operating MFSs at varying feed water flow rates. Short-term (9 days) biofouling studies were carried out with nutrient dosage to the MFS feed water to accelerate the biofouling rate. Long-term (96 days) biofouling studies were done without nutrient dosage to the MFS feed water. Feed channel pressure drop was monitored and accumulation of active biomass was quantified by adenosine tri phosphate (ATP) determination. The six feed spacers were ranked on pressure drop (hydraulic characterization) and on biofouling impact (biofouling studies). Significantly different trends in hydraulic resistance and biofouling impact for the six feed spacers were observed. The same ranking for biofouling impact on the feed spacers was found for the (i) short-term biofouling study with nutrient dosage and the (ii) long-term biofouling study without nutrient dosage. The ranking for hydraulic resistance for six virgin feed spacers differed significantly from the ranking of the biofouling impact, indicating that hydraulic resistance of clean feed spacers does not predict the hydraulic resistance of biofouled feed spacers. Better geometric design of feed spacers can be a suitable approach to minimize impact of biofouling in spiral wound membrane systems.

Impact of organic nutrient load on biomass accumulation, feed channel pressure drop increase and permeate flux decline in membrane systems.

The influence of organic nutrient load on biomass accumulation (biofouling) and pressure drop development in membrane filtration systems was investigated. Nutrient load is the product of nutrient concentration and linear flow velocity. Biofouling - excessive growth of microbial biomass in membrane systems - hampers membrane performance. The influence of biodegradable organic nutrient load on biofouling was investigated at varying (i) crossflow velocity, (ii) nutrient concentration, (iii) shear, and (iv) feed spacer thickness. Experimental studies were performed with membrane fouling simulators (MFSs) containing a reverse osmosis (RO) membrane and a 31 mil thick feed spacer, commonly applied in practice in RO and nanofiltration (NF) spiral-wound membrane modules. Numerical modeling studies were done with identical feed spacer geometry differing in thickness (28, 31 and 34 mil). Additionally, experiments were done applying a forward osmosis (FO) membrane with varying spacer thickness (28, 31 and 34 mil), addressing the permeate flux decline and biofilm development. Assessed were the development of feed channel pressure drop (MFS studies), permeate flux (FO studies) and accumulated biomass amount measured by adenosine triphosphate (ATP) and total organic carbon (TOC). Our studies showed that the organic nutrient load determined the accumulated amount of biomass. The same amount of accumulated biomass was found at constant nutrient load irrespective of linear flow velocity, shear, and/or feed spacer thickness. The impact of the same amount of accumulated biomass on feed channel pressure drop and permeate flux was influenced by membrane process design and operational conditions. Reducing the nutrient load by pretreatment slowed-down the biofilm formation. The impact of accumulated biomass on membrane performance was reduced by applying a lower crossflow velocity and/or a thicker and/or a modified geometry feed spacer. The results indicate that cleanings can be delayed but are unavoidable.

In-situ biofilm characterization in membrane systems using Optical Coherence Tomography: formation, structure, detachment and impact of flux change.

Biofouling causes performance loss in spiral wound nanofiltration (NF) and reverse osmosis (RO) membrane operation for process and drinking water production. The development of biofilm formation, structure and detachment was studied in-situ, non-destructively with Optical Coherence Tomography (OCT) in direct relation with the hydraulic biofilm resistance and membrane performance parameters: transmembrane pressure drop (TMP) and feed-channel pressure drop (FCP). The objective was to evaluate the suitability of OCT for biofouling studies, applying a membrane biofouling test cell operated at constant crossflow velocity (0.1 m s(-1)) and permeate flux (20 L m(-2)h(-1)). In time, the biofilm thickness on the membrane increased continuously causing a decline in membrane performance. Local biofilm detachment was observed at the biofilm-membrane interface. A mature biofilm was subjected to permeate flux variation (20 to 60 to 20 L m(-2)h(-1)). An increase in permeate flux caused a decrease in biofilm thickness and an increase in biofilm resistance, indicating biofilm compaction. Restoring the original permeate flux did not completely restore the original biofilm parameters: After elevated flux operation the biofilm thickness was reduced to 75% and the hydraulic resistance increased to 116% of the original values. Therefore, after a temporarily permeate flux increase the impact of the biofilm on membrane performance was stronger. OCT imaging of the biofilm with increased permeate flux revealed that the biofilm became compacted, lost internal voids, and became more dense. Therefore, membrane performance losses were not only related to biofilm thickness but also to the internal biofilm structure, e.g. caused by changes in pressure. Optical Coherence Tomography proved to be a suitable tool for quantitative in-situ biofilm thickness and morphology studies which can be carried out non-destructively and in real-time in transparent membrane biofouling monitors.

Impact of biofilm accumulation on transmembrane and feed channel pressure drop: effects of crossflow velocity, feed spacer and biodegradable nutrient.

Biofilm formation causes performance loss in spiral-wound membrane systems. In this study a microfiltration membrane was used in experiments to simulate fouling in spiral-wound reverse osmosis (RO) and nanofiltration (NF) membrane modules without the influence of concentration polarization. The resistance of a microfiltration membrane is much lower than the intrinsic biofilm resistance, enabling the detection of biofilm accumulation in an early stage. The impact of biofilm accumulation on the transmembrane (biofilm) resistance and feed channel pressure drop as a function of the crossflow velocity (0.05 and 0.20 m s(-1)) and feed spacer presence was studied in transparent membrane biofouling monitors operated at a permeate flux of 20 L m(-2) h(-1). As biodegradable nutrient, acetate was dosed to the feed water (1.0 and 0.25 mg L(-1) carbon) to enhance biofilm accumulation in the monitors. The studies showed that biofilm formation caused an increased transmembrane resistance and feed channel pressure drop. The effect was strongest at the highest crossflow velocity (0.2 m s(-1)) and in the presence of a feed spacer. Simulating conditions as currently applied in nanofiltration and reverse osmosis installations (crossflow velocity 0.2 m s(-1) and standard feed spacer) showed that the impact of biofilm formation on performance, in terms of transmembrane and feed channel pressure drop, was strong. This emphasized the importance of hydrodynamics and feed spacer design. Biomass accumulation was related to the nutrient load (nutrient concentration and linear flow velocity). Reducing the nutrient concentration of the feed water enabled the application of higher crossflow velocities. Pretreatment to remove biodegradable nutrient and removal of biomass from the membrane elements played an important part to prevent or restrict biofouling.

A novel scenario for biofouling control of spiral wound membrane systems.

Current strategies to control biofouling in nanofiltration and reverse osmosis membrane systems such as chemical cleaning and use of low fouling membranes are not always successful. Based on recent studies, an alternative approach is derived, combining a lower linear flow velocity in lead modules and adapted designs for feed spacer with an advanced cleaning strategy. This approach can be realized by small adaptations in current plant design. A lower linear flow velocity in lead spiral wound membrane modules results in (i) lower energy use, (ii) lower impact of biomass on the feed channel pressure drop, and (iii) more fluffy biofilm that may be easier to remove from the lead membrane modules, especially when adapted feed spacers combined with a reversed enhanced flush are applied. This rational scenario can result in effective biofouling control at low energy requirements, minimal chemical use and minimal cost.

Integrated approach for biofouling control.

Despite extensive research efforts, past and present strategies to control biofouling problems in spiral-wound nanofiltration and reverse osmosis membranes have not been successful under all circumstances. Gaining insight in the biofouling process is a first necessity. Based on recent insights, an overview is given of 12 potential complementary approaches to solve biofouling. Combinations of approaches may be more efficient in biofouling control than a single approach. A single approach must be 100% effective, while in combination each individual approach can be partially effective while the combination is still efficient. An integrated Approach for Biofouling Control (ABC) is proposed, based on three corner stones: (i) equipment design and operation, (ii) biomass growth conditions, and (iii) cleaning agents as a framework to control biofouling. While past and present strategies addressed mainly membranes and microorganisms, i.e. removal or inactivation of biomass, this ABC-approach addresses the total membrane filtration system. It is anticipated that this integral approach will enable a more rational and effective control of biofouling. Although in this stage chemical cleaning and biofouling inhibitor dosage seem unavoidable to control biofouling, it is expected that in future--because of sustainability and costs reasons--membrane systems will be developed without or with minimal need for chemical cleaning and dosing. Three potential scenarios for biofouling control are proposed based on (i) biofouling tolerant spiral wound membrane systems, (ii) capillary membranes, and (iii) phosphate limitation.

Phosphate limitation to control biofouling.

Phosphate limitation as a method to control biofouling of spiral wound reverse osmosis (RO) membranes was studied at a full-scale installation fed with extensively pretreated water. The RO installation is characterized by (i) a low feed channel pressure drop increase and (ii) low biomass concentrations in membrane elements at the installation feed side. This installation contrasted sharply with installations fed with less extensively pretreated feed water (and therefore higher phosphate concentrations) experiencing a high-pressure drop increase and high biomass concentrations in lead elements. Membrane fouling simulator (MFS) studies showed that low phosphate concentrations (approximately 0.3 microg P L(-1)) in the feed water restricted the pressure drop increase and biomass accumulation, even at high substrate (organic carbon) concentrations. In the MFS under ortho-phosphate limiting conditions, dosing phosphonate based antiscalants caused biofouling while no biofouling was observed when acids or phosphonate-free antiscalants were used. Antiscalant dosage could increase both phosphate and substrate concentrations of the water. Therefore, antiscalant selection may be critical for biofouling control. Since no biofouling was observed at low phosphate concentrations, restricting biomass growth by phosphate limitation may be a feasible approach to control biofouling, even in the presence of high organic carbon levels.

Impact of flow regime on pressure drop increase and biomass accumulation and morphology in membrane systems.

Biomass accumulation and pressure drop development have been studied in membrane fouling simulators at different flow regimes. At linear flow velocities as applied in practice in spiral wound nanofiltration (NF) and reverse osmosis (RO) membranes, voluminous and filamentous biofilm structures developed in the feed spacer channel, causing a significant increase in feed channel pressure drop. Elevated shear by both single phase flow (water) and two phase flow (water with air sparging: bubble flow) caused biofilm filaments and a pressure drop increase. The amount of accumulated biomass was independent of the applied shear, depending on the substrate loading rate (product of substrate concentration and linear flow velocity) only. The biofilm streamers oscillated in the passing water. Bubble flow resulted in a more compact and less filamentous biofilm structure than single phase flow, causing a much lower pressure drop increase. The biofilm grown under low shear conditions was more easy to remove during water flushing compared to a biofilm grown under high shear. To control biofouling, biofilm structure may be adjusted using biofilm morphology engineering combined with biomass removal from membrane elements by periodic reverse flushing using modified feed spacers. Potential long and short term consequences of flow regimes on biofilm development are discussed. Flow regimes manipulate biofilm morphology affecting membrane performance, enabling new approaches to control biofouling.

Pressure drop increase by biofilm accumulation in spiral wound RO and NF membrane systems: role of substrate concentration, flow velocity, substrate load and flow direction.

In an earlier study, it was shown that biofouling predominantly is a feed spacer channel problem. In this article, pressure drop development and biofilm accumulation in membrane fouling simulators have been studied without permeate production as a function of the process parameters substrate concentration, linear flow velocity, substrate load and flow direction. At the applied substrate concentration range, 100-400 microg l(-1) as acetate carbon, a higher concentration caused a faster and greater pressure drop increase and a greater accumulation of biomass. Within the range of linear flow velocities as applied in practice, a higher linear flow velocity resulted in a higher initial pressure drop in addition to a more rapid and greater pressure drop increase and biomass accumulation. Reduction of the linear flow velocity resulted in an instantaneous reduction of the pressure drop caused by the accumulated biomass, without changing the biofilm concentration. A higher substrate load (product of substrate concentration and flow velocity) was related to biomass accumulation. The effect of the same amount of accumulated biomass on the pressure drop increase was related to the linear flow velocity. A decrease of substrate load caused a gradual decline in time of both biomass concentration and pressure drop increase. It was concluded that the pressure drop increase over spiral wound reverse osmosis (RO) and nanofiltration (NF) membrane systems can be reduced by lowering both substrate load and linear flow velocity. There is a need for RO and NF systems with a low pressure drop increase irrespective of the biomass formation. Current efforts to control biofouling of spiral wound membranes focus in addition to pretreatment on membrane improvement. According to these authors, adaptation of the hydrodynamics, spacers and pressure vessel configuration offer promising alternatives. Additional approaches may be replacing heavily biofouled elements and flow direction reversal.

Biofouling of spiral-wound nanofiltration and reverse osmosis membranes: a feed spacer problem.

Biofouling was studied in full-scale and pilot-scale installations, test-rigs and membrane fouling monitors by conventional methods as well as Magnetic Resonance Imaging (MRI). Independent of permeate production, the feed spacer channel pressure drop and biomass concentration increased similarly in a nanofiltration pilot installation. In the presence of a feed spacer the absolute feed channel pressure drop increase caused by biomass accumulation was much higher than when a feed spacer was absent: in both spiral-wound nanofiltration and reverse osmosis systems biofouling is dominantly a feed spacer problem. This conclusion is based on (i) in-situ visual observations of the fouling accumulation, (ii) in-situ non-destructive observations of the fouling accumulation and velocity distribution profiles using MRI, and (iii) differences in pressure drop and biomass development in monitors with and without feed spacer. MRI studies showed that even a restricted biofilm accumulation on the feed channel spacer influenced the velocity distribution profile strongly. Biofouling control should be focused on the development of low fouling feed spacers and hydrodynamic conditions to restrict the impact of biomass accumulation on the feed channel pressure drop increase.

Quantitative biofouling diagnosis in full scale nanofiltration and reverse osmosis installations.

Biofilm accumulation in nanofiltration and reverse osmosis membrane elements results in a relative increase of normalised pressure drop (DeltaNPD). However, an increase in DeltaNPD is not exclusively linked to biofouling. In order to quantify biofouling, the biomass parameters adenosine triphosphate (ATP), total cell count and heterotrophic plate count in membrane elements were investigated during membrane autopsies and compared with DeltaNPD in test rigs and 15 full scale investigations with different types of feed water. The combination of biomass related parameters ATP and total cell count in membrane elements seem to be suitable parameters for diagnosis of biofouling, whereas plate counts were not appropriate to assess biofouling. The applied DeltaNPD measurement was too insensitive for early detection of fouling. Measurements of biological parameters in the water were shown to be not appropriate in quantifying biofouling. Evidently, there is a need for a practical tool, sensitive pressure drop data and systematic research.

The membrane fouling simulator: a suitable tool for prediction and characterisation of membrane fouling.

A new tool--the Membrane Fouling Simulator (MFS)--is developed to measure membrane fouling (pressure drop increase) in a small and simple system, representative for spiral wound membranes applied in water treatment. With the MFS, fouling development can be monitored systematically by (i) pressure drop, (ii) in situ and non-destructive (visual) observations using the sight glass and (iii) analysis of coupons sampled from the membrane sheet in the MFS. A comparison study of the MFS with spiral wound membrane elements (test rigs and a full scale installation) showed the same fouling. The MFS provided reproducible data. The small size and low water and chemical use of the MFS facilitate to perform systematic parallel studies. With the MFS, fouling of membranes applied in water treatment can be characterised.

The influence of water treatment processes on the presence of organic surrogates and mutagenic compounds in water.

The effects of granular activated carbon filtration and of the combination of ozonation and GAC filtration on the quality of Rhine water were studied in a pilot plant. The scope of the study was to compare both systems in relation to the removal of organic contaminants in water, and to the reduction of the side effects of chlorination. The water quality was measured with organic surrogate parameters (organohalogen, -nitrogen, -phosphorus and -sulphur) and in bacterial mutagenicity assays. In this particular setting, the combination of ozonation and GAC filtration was superior in all points to GAC filtration alone. The effects of ozonation are sometimes quite different, depending on the type of water treated. Its positive influence should be confirmed in a local situation. As GAC treatment causes a shift towards formation of more brominated THM after chlorination, special attention was given to this item. A higher inorganic bromide/DOC ratio resulted in higher brominated THM concentrations after chlorination. However, the mutagens formed during chlorination in presence of more inorganic bromide could be inactivated more easily by rat liver homogenate than in the normal setting. The results of this study confirmed earlier findings stating a negative influence of chlorination on water quality.