Recent advances in membrane bioreactors (MBRs): Membrane fouling and membrane material

Membrane bioreactors (MBRs) have been actively employed for municipal and industrial wastewater treatments. So far, membrane fouling and the high cost of membranes are main obstacles for wider application of MBRs. Over the past few years, considerable investigations have been performed to understand MBR fouling in detail and to develop high-flux or low-cost membranes. This review attempted to address the recent and current developments in MBRs on the basis of reported literature in order to provide more detailed information about MBRs. In this paper, the fouling behaviour, fouling factors and fouling control strategies were discussed. Recent developments in membrane materials including low-cost filters, membrane modification and dynamic membranes were also reviewed. Lastly, the future trends in membrane fouling research and membrane material development in the coming years were addressed.     

Extracellular polymeric substances (EPS) properties and their effects on membrane fouling in a submerged membrane bioreactor

A pilot-scale submerged membrane bioreactor (MBR) for real municipal wastewater treatment was operated for over one year in order to investigate extracellular polymeric substances (EPS) properties and their role in membrane fouling. The components and properties of bound EPS were examined by the evaluation of mean oxidation state (MOS) of organic carbons, Fourier transform infrared (FT-IR) spectroscopy, three-dimensional excitation-emission matrix (EEM) fluorescence spectroscopy, and gel filtration chromatography (GFC), etc. Test results showed that MOS of organic carbons in the bound EPS was ranging from −0.14 to −0.51, and major components could be assessed as proteins and carbohydrates. FT-IR analysis confirmed the presence of proteins and carbohydrates in the bound EPS. The organic substances with fluorescence characteristics in the bound EPS were identified as proteins, visible humic acid-like substances and fulvic acid-like substances by EEM technology. GFC analysis demonstrated that EPS had part of higher MW molecules and a broader MW distribution than the influent wastewater. It was also found that a high shear stress imposed on mixed liquor could result in the release of EPS, which would in turn influence membrane fouling in MBRs. Bound EPS solution was observed to have a stronger potential of fouling than mixed liquor. During long-term operation of the MBR, bound EPS demonstrated positive correlations with membrane fouling while temperature was verified as a negative factor affecting EPS concentration. Compared to tightly bound EPS (TB-EPS), loosely bound EPS (LB-EPS) showed more significant correlations with membrane fouling. This critical investigation would contribute towards a better understanding of the behavior, composition and fouling potential of EPS in MBR operation.     

A comparison of membrane fouling under constant and variable organic loadings in submerge membrane bioreactors

The aim of this study is to compare the effect of constant and variable influent organic loadings on membrane fouling in submerged membrane bioreactors (sMBRs). Two identical lab-scale sMBRs were operated for 162 days at an SRT of 30 days, whereas the influent organic loading was kept constant in one MBR, and varied in another. The microbial characteristics of sludge in terms of MLSS, bound EPS, EPS in the supernatant and particle size distribution were investigated in order to evaluate their respective effect on membrane fouling. During the start-up period, membrane fouling in the MBR fed with variable loadings was more serious than that in the MBR with the constant loading. However, at the stable state, the fouling tendency was clearly reversed with less membrane fouling for variable feed strength. It was shown that the contents of polysaccharides in the supernatant and particle size of the bioflocs were responsible for the observed differences in the fouling tendencies of the two MBRs.     

Influence of mixed liquor properties and aeration intensity on membrane fouling in a submerged membrane bioreactor at high mixed liquor suspended solids concentrations

This paper presents the results of 195 days of pilot-scale submerged membrane bioreactor (SMBR) experiments on settled municipal wastewater. Short-term and long-term thickening experiments were performed at a constant membrane flux of 30L/(m(2)h) to determine the impact of the following mixed liquor properties: colloidal material, soluble COD, soluble microbial products, extracellular polymeric substances, and viscosity along with aeration intensity on membrane fouling at high mixed liquor suspended solids (MLSS) concentrations. The normalized permeability declined with increasing MLSS concentrations in all experiments and increasing the coarse bubble aeration intensity increased the permeability at a given MLSS concentration. Using a dynamic approach, this work demonstrates the importance of mixed liquor viscosity, which impacts the efficacy of the coarse bubble aeration, in sustaining membrane permeability. Over an extended thickening time period, a small increase in MLSS concentration and mixed liquor viscosity becomes more prevalent and leads to greater permeability decline at a given MLSS concentration.     

Characterization of the size-fractionated biomacromolecules: tracking their role and fate in a membrane bioreactor

This article presents a study aimed at the fractionation and characterization of what is thought to be one of the most complex organic mixtures produced by activated sludge: biomacromolecules (BMM). Photometric quantification combined with excitation-emission matrix (EEM) fluorescence spectroscopy and nuclear magnetic resonance (NMR) measurements were used to characterize BMM in a membrane bioreactor (MBR) from a chemical perspective. Overall, the BMM in sludge supernatant were mainly present in three fractions: colloidal BMM (BMM_c, >0.45 μm), biopolymeric BMM (BMM_b, 0.45 μm-100 kDa) and low molecular weight (MW) fraction (<5 kDa). The analysis of fluorescence regional integration (FRI) showed that the organics in membrane permeate and those in the low-MW fraction of sludge supernatant were of similar chemical composition. The characterization by NMR suggested that the BMM_c fraction had similar carbon content of proteins and polysaccharides. In contrast, the BMM_b and the low-MW BMM were proved to be carbonaceous and aromatics, respectively. Moreover, because of the high MW and gelling property, polysaccharides were found to have a high potential to accumulate on the membranes. In addition, the lipids present in the BMM_b of the sludge supernatant were demonstrated to be another important foulant due to their large size. Our results also indicated that aromatic proteins had a higher fouling propensity than tryptophan proteins though they were of similar size nature. This work could be useful for better understanding of the chemical nature of BMMs in MBRs.     

Submerged anaerobic membrane bioreactor for low-strength wastewater treatment: Effect of HRT and SRT on treatment performance and membrane fouling

Three 6-L submerged anaerobic membrane bioreactors (SAnMBRs) with solids retention times (SRTs) of 30, 60 and infinite days were setup for treating synthetic low-strength wastewater at hydraulic retention times (HRTs) of 12, 10 and 8 h. Total COD removal efficiencies higher than 97% were achieved at all operating conditions. Maximum biogas production rate was 0.056 L CH₄/g MLVSS d at an infinite SRT. A shorter HRT or longer SRT increased biogas production due to increased organic loading rate or enhanced dominancy of methanogenics. A decrease in HRT enhanced growth of biomass and accumulation of soluble microbial products (SMP), which accelerated membrane fouling. A drop in carbohydrate to protein ratio also inversely affected fouling. At 12-h HRT, the effect of SRT on biomass concentration in SAnMBRs was negligible and membrane fouling was controlled by variant surface modification due to different SMP compositions, i.e., higher carbohydrate and protein concentrations in SMP at longer SRT resulted in higher membrane fouling rate. At 8 and 10-h HRTs, infinite SRT in SAnMBR caused highest MLSS and SMP concentrations, which sped up particle deposition and biocake/biofilm development. At longer SRT, lower extracellular polymeric substances reduced flocculation of particulates and particle sizes, further aggravated membrane fouling.     

Characterization of dissolved extracellular organic matter (dEOM) and bound extracellular organic matter (bEOM) of Microcystis aeruginosa and their impacts on UF membrane fouling

Extracellular organic matter (EOM) of cyanobacteria was classified into the dissolved EOM (dEOM) which was released into culture solution and the bound EOM (bEOM) which surrounded the cells. The dEOM and bEOM extracted from Microcystis aeruginosa in stationary phase were used to study their characteristic differences and then their impacts on ultrafiltration (UF) membrane fouling. Component analyses showed that dEOM was comprised of proteins, polysaccharides and humic-like substances, while that bEOM contained only proteins and polysaccharides. Additionally, polysaccharides dominated in dEOM with a polysaccharide/DOC ratio of 1.11 mg mg⁻¹, while proteins were the primary components of bEOM with a protein/DOC ratio of 1.08 mg mg⁻¹. Results of size fractionation and XAD resin fractionation revealed that bEOM was mainly distributed in the high-MW and hydrophobic fractions, while that dEOM was more hydrophilic. Result of UF experiments indicated that dEOM which had a higher organic content and stronger hydrophilicity caused more severe flux decline and reversible fouling, and that bEOM led to slower flux decline but more irreversible fouling due to less electrostatic repulsive and more hydrophobic adhesion. The impacts of these two kinds of EOM on the UF fouling caused by cyanobacterial cells were also investigated. It was found that both flux decline and irreversible membrane fouling caused by the cells were aggravated when cells were together with EOM, especially for bEOM which might increase the surface hydrophobicity of the cells.     

Sludge properties and their effects on membrane fouling in submerged anaerobic membrane bioreactors (SAnMBRs)

Two submerged anaerobic membrane bioreactors (SAnMBRs) (thermophilic vs. mesophilic) were operated for a period of 3.5 months with kraft evaporator condensate at a feed chemical oxygen demand of 10,000 mg/L. The results show that the filtration behavior of the two systems was significantly different. The filtration resistance in the thermophilic SAnMBR was about 5–10 times higher than that of the mesophilic system when operated under similar hydrodynamic conditions. Comparison of sludge properties and cake layer structure from the two systems was made to elucidate major factors governing the different filtration characteristics. There were more soluble microbial products (SMP) and biopolymer clusters (BPC) produced and a larger portion of fine flocs (<15 μm) in the thermophilic SAnMBR. Analysis of bound extracellular polymeric substances (EPS) showed that the thermophilic sludge had a higher protein/polysaccharide ratio in EPS, as compared to that in the mesophilic sludge. A series of analyses, including Fourier transform infrared (FTIR) spectroscopy, energy dispersive X-ray spectroscopy (EDX), confocal laser scanning microscopy (CLSM), scanning electron microscopy (SEM), atomic force microscopy (AFM) and particle size analyzer showed that the cake layer formed in the thermophilic SAnMBR contained higher levels of both organic and inorganic foulants, smaller particle sizes, and especially, a denser and more compact sludge cake structure. These results indicate that floc size, SMP, BPC, bound EPS as well as cake layer structure are the major factors governing membrane fouling in SAnMBR systems.     

A comparative study of fouling-related properties of sludge from conventional and membrane enhanced biological phosphorus removal processes

The physical and biochemical properties of activated sludge mixed liquor, including floc size distribution, zeta potential, relative hydrophobicity, and bound and unbound (soluble) extracellular polymeric substances (EPS), were examined in this study to evaluate their relationship to membrane fouling. Mixed liquors from a membrane enhanced biological phosphorus removal (MEBPR) process and a conventional enhanced biological phosphorus removal (CEBPR) process were compared. It was found that the floc size distribution and the amount of soluble EPS in the mixed liquor were the most important properties that significantly influenced the fouling propensity of sludge. Contrary to the literature, the content of EPS bound in activated sludge flocs was not found to be directly associated with membrane fouling, and sludge surface properties such as zeta potential and relative hydrophobicity were not closely related to the observed differences in the fouling tendencies of the two types of sludge.     

Occurrence and composition of extracellular lipids and polysaccharides in a full-scale membrane bioreactor

The aim of this study was to characterize the polysaccharides and lipid fractions of membrane foulants in a full-scale membrane bioreactor (MBR) treating municipal wastewater. Both of these polymeric compounds are major components of bacterial lipopolysaccharides and are impacting membrane fouling; however most of the data so far have been collected by determining sum parameters rather than the detailed composition of these polymers.Photometric analysis of sugars showed that uronic acids (glucuronic, mannuronic and galacturonic acid) as common units of bacterial polysaccharides accounted for 8% (w/w) of extracellular polymeric substances (EPS) in activated sludge flocs. Further the so-called polysaccharide peak of EPS, with a molecular weight >10 kDa according to size exclusion chromatography, was proven to contain bacterial sugar units as shown by high resolution LC-MS. Interestingly, only traces of uronic acids could be detected in EPS of the membrane fouling layer.A far more dramatic enrichment in the fouling layer was revealed for the lipid fraction of EPS, which was determined as fatty acid methyl esters by GC-MS. The weight percentage of fatty acids in EPS extracted from fouled ultrafiltration membranes was much higher (10%) than in the activated sludge itself (1-3%). The fatty acids accumulated on the membrane fouling layer were obviously not only of microbial origin (C16:0, C18:0) but also derived from the raw wastewater itself (C9:0). Hydrophobic interaction of lipids with the PVDF (polyvinylidene fluoride) membrane material therefore seems a plausible explanation for the observed fouling phenomenon. The results suggest that fatty acids from bacterial lipopolysaccharides as well as from synthetic sources are of much higher relevance to membrane fouling than previously assumed.     

Effects of mass retention of dissolved organic matter and membrane pore size on membrane fouling and flux decline

Ultrafiltration (UF) fouling has been attributed to concentration polarization, gel layer formation as well as outer and inner membrane pore clogging. It is believed that mass of humic materials either retained on membrane surface or associated with membrane inner pore surface is the primary cause for permeate flux decline and filtration resistance build-up in water supply industries. While biofilm/biofouling and inorganic matter could also be contributing factors for permeability decline in wastewater treatment practices. The present study relates UF fouling to mass of dissolved organic matter (DOM) retained on membrane and quantifies the effect of retained DOM mass on filtration flux decline. The results demonstrate that larger pore membranes exhibit significant flux decline in comparison with the smaller ones. During a 24-h period, dissolved organic carbon mass retained in 10 kDa membranes was about 1.0 g m⁻² and that in 100 kDa membranes was more than 3 times higher (3.6 g m⁻²). The accumulation of retained DOM mass significantly affects permeate flux. It is highly likely that some DOMs bind or aggregate together to form surface gel layer in the smaller 10 kDa UF system; those DOMs largely present in inner pore and serving as pore blockage on a loose membrane (100 kDa) are responsible for severe flux decline.     

Post-treatment of upflow anaerobic sludge blanket effluent by combining the membrane filtration process: fouling control by intermittent permeation and air sparging

In this study, the membrane filtration process was proposed as a post-treatment process to treat the upflow anaerobic sludge blanket (UASB) effluent. The flat-sheet membrane modules were submerged into the UASB reactor to retain the suspended solids in the UASB effluent under intermittent permeation and air sparging conditions. The results indicated that intermittent permeation enhanced the sustainability of the submerged membrane and an idle time of 4 min with a 10-min filtration was optimal for reducing membrane fouling under the experimental conditions. Air sparging could also alleviate membrane fouling, and the lowest transmembrane pressure (TMP) change rate (dTMP/d t ) was achieved at the moderate aeration rate of 2 L/min. It appears to be effective to alleviate membrane fouling and achieve high effluent production at a flux of 25 L/m² h and an idle time of 4 min with a 10-min filtration considering the energy consumption.     

Influence of shear on the production of extracellular polymeric substances in membrane bioreactors

Shear is used to control fouling in membrane bioreactor (MBR) systems. However, shear also influences the physicochemical and biological properties of MBR biomass. The current study examines the relationship between the level of shear and extracellular polymeric substance (EPS) production in MBRs. Two identical MBRs were operated in parallel where the biomass in one reactor was exposed to seven times greater shear forces. The concentrations of floc-associated and soluble EPS were monitored for the duration of the experiment. The stickiness of extracted floc-associated EPS from each reactor was also characterized using atomic force microscopy. A mathematical model of floc-associated and soluble EPS production was applied to quantitatively describe changes in EPS production with shear. Biomass grown in a high shear environment has lower floc-associated EPS production compared to biomass grown in a lower shear environment. This decrease in floc-associated EPS production also corresponds to a decrease in soluble EPS production, which can be explained by both the lower concentration of floc-associated EPS and the production of stickier floc-associated EPS that is more erosion resistant in the high shear reactor. This research suggests that mechanical stresses can have a significant impact on the production rates of floc-associated and soluble EPS—key parameters governing membrane fouling in MBRs.     

Granular iron oxide adsorbents to control natural organic matter and membrane fouling in ultrafiltration water treatment

Fine iron oxide particles (IOPs) are effective in removing natural organic matter (NOM) that causes membrane fouling in water treatment, but the separation of used IOPs is problematic. This study focused on the fabrication and use of granular iron oxide adsorbents, in combination with ultrafiltration (UF) membranes while investigating the NOM removal efficiency and fouling control. Sulfonated styrene-divinylbenzene copolymer beads were coated with two types of iron oxides (ferrihydrite and magnetite) and their performances were compared to that of fine IOPs. A significant amount of iron oxide coating (52–63 mg of Fe per g bead) was achieved by means of electrostatic binding and hydrolysis of iron ions. Iron oxide coated polymer (IOCP) beads were able to remove some amounts (～20%) of dissolved organic carbon (DOC) comparable to that achieved by IOPs within a short period of time (<15 min). Regenerated IOCPs exhibited the same sorption capacity as the fresh ones. The integrated IOCP/UF system operation with a 15-min empty bed contact time and 10-h cyclic regeneration maintained the 20% DOC removal with no sign of significant membrane fouling. In contrast, a sharp transmembrane pressure buildup occurred in the UF system when no iron oxide pretreatment was applied, regardless of the types of membranes tested. Iron oxide adsorbed the NOM fraction with molecular weights of >1000 kDa which is believed to be responsible for severe UF fouling.     

Ultrafiltration membrane fouling by extracellular organic matters (EOM) of Microcystis aeruginosa in stationary phase: influences of interfacial characteristics of foulants and fouling mechanisms

This paper focused on the membrane fouling caused by extracellular organic matters (EOM) which was extracted from lab-cultured Microcystis aeruginosa in stationary phase. The characteristics of EOM such as molecular weight distribution, hydrophobicity and fluorescence were measured. It was found that high molecular weight (MW) and hydrophilic organics accounted for the major parts of algal EOM which was comprised of protein-like, polysaccharide-like and humic-like substances. Ultrafiltration (UF) experiments were carried out in a stirring cell and hydrophobic polyethersulfone (PES) membranes which carried negative charge were used. Prefiltration, calcium addition and XAD fractionation were employed to change the interfacial characteristics of EOM. Then the effects of these interfacial characteristics on flux decline, reversibility and mass balance of organics were compared. Algal EOM proved to cause serious membrane fouling during UF. The fraction of algal EOM between 0.45 μm and 100 kDa contributed a significant portion of the fouling. Hydrophobic organics in EOM tended to adhere to membrane surface causing irreversible fouling, while the cake layer formed by hydrophilic organics caused greater resistance to water flow due to hydrophilic interaction such as hydrogen bond and led to faster flux decline during UF. The results also indicated that the algal EOM was negatively charged and the electrostatic repulsion could prevent organics from adhering to membrane surface. In term of fouling mechanisms, cake layer formation, hydrophobic adhesion and pore plugging were the main mechanisms for membrane fouling caused by algal EOM.     

Composition of a protein-like fluorophore of dissolved organic matter in coastal wetland and estuarine ecosystems

This study demonstrates the compositional heterogeneity of a protein-like fluorescence emission signal (T-peak; excitation/emission maximum at 280/325 nm) of dissolved organic matter (DOM) samples collected from subtropical river and estuarine environments. Natural water samples were collected from the Florida Coastal Everglades ecosystem. The samples were ultrafiltered and excitation-emission fluorescence matrices were obtained. The T-peak intensity correlated positively with N concentration of the ultrafiltered DOM solution (UDON), although, the low correlation coefficient (r(2)=0.140, p<0.05) suggested the coexistence of proteins with other classes of compounds in the T-peak. As such, the T-peak was unbundled on size exclusion chromatography. The elution curves showed that the T-peak was composed of two compounds with distinct molecular weights (MW) with nominal MWs of about >5 x 10(4) (T(1)) and approximately 7.6 x 10(3) (T(2)) and with varying relative abundance among samples. The T(1)-peak intensity correlated strongly with [UDON] (r(2)=0.516, p<0.001), while T(2)-peak did not, which suggested that the T-peak is composed of a mixture of compounds with different chemical structures and ecological roles, namely proteinaceous materials and presumably phenolic moieties in humic-like substances. Natural source of the latter may include polyphenols leached from senescent plant materials, which are important precursors of humic substances. This idea is supported by the fact that polyphenols, such as gallic acid, an important constituent of hydrolysable tannins, and condensed tannins extracted from red mangrove (Rhizophora mangle) leaves exhibited the fluorescence peak in the close vicinity of the T-peak (260/346 and 275/313 nm, respectively). Based on this study the application of the T-peak as a proxy for [DON] in natural waters may have limitations in coastal zones with significant terrestrial DOM input.     

Identification and quantification of major organic foulants in treated domestic wastewater affecting filterability in dead-end ultrafiltration

Ultrafiltration (UF) membranes can be used after conventional wastewater treatment to produce particle free and hygienically safe water for reuse. However, membrane fouling affects the performance of UF to a large extent. Stirred cell tests with UF membrane show high flux decline filtering treated domestic wastewater. Investigation on the impact of size fractioned substances indicates that dissolved substances are major foulants affecting water filterability. Dissolved organic substances in feed and permeate samples of the stirred cell tests are analyzed by liquid chromatography with online organic carbon detection (LC-OCD). The resulting chromatograms displayed a significant difference of feed and permeate samples in the range of large molecules identified as biopolymer peak. The substances detected in this peak (mostly macro polysaccharide-like and protein-like molecules) are almost completely retained by UF membranes. Quantified investigation shows that biopolymer concentration influences filterability of corresponding water sample proportionally. The apparent magnitude of delivered biopolymer to membrane has a striking correlation with fouling resistance. The relationship was verified to be reproducible using different water samples. Mechanism analysis demonstrates that based on the delivered biopolymer load to membrane pore blocking or cake/gel fouling is the main fouling mechanism in the present experiment conditions.     

Impact of feed water acidification with weak and strong acids on colloidal silica fouling in ultrafiltration membrane processes

Although acidification of feed water is a common practice to prevent scaling of the sparingly soluble minerals in nanofiltration and reverse osmosis processes, the change of acidity may have a potentially adverse impact on colloidal fouling, which is another important type of fouling on the membranes. In this paper, commonly used strong and weak acids are quantitatively investigated for their effect on colloidal silica fouling with a lab-scale ultrafiltration (UF) membrane system. Experiments showed that addition of either strong or weak acids in feed water would intensify colloidal fouling. However, the strength of colloidal fouling with strong acid addition was consistently higher (12-37%) than that with weak acid addition at pH 3. The smaller increase in colloidal fouling potential observed with weak acids was attributed to the adsorption of weak acid anions on the colloidal silica surface, which kept the absolute value of zeta potential of the colloids relatively high. Consequently, the difference in colloidal fouling potential with the additions of strong and weak acids diminished at high salt concentration. The findings implied that the type of acid used in feed water acidification could have a significant impact on colloidal fouling for low-salinity waters.     

Impact of coagulation and adsorption on DOC fractions of secondary effluent and resulting fouling behaviour in ultrafiltration

Membrane fouling by macromolecular dissolved organic compounds is still a fundamental drawback in low-pressure membrane filtration of secondary effluent. In this study, pre-treatment of secondary effluent by coagulation and/or adsorption was investigated in terms of removal of different dissolved organic carbon (DOC) fractions, especially macromolecular substances. DOC fractionation has been characterised by size exclusion chromatography. Adsorption tests using four commercially available activated carbons yielded a removal of small as well as larger organic compounds, revealing differences in the affinity towards macromolecules depending on the type of applied activated carbon. By contrast, coagulation removed predominantly larger molecules, i.e., biopolymers and humic substances. In terms of DOC reduction, the coagulant ferric chloride was superior to aluminium chloride. A combination of coagulation and adsorption resulted in the addition of individual removal efficiencies, suggesting that different fractions of organic compounds were involved in each of the processes. After removal of macromolecular organic compounds either by coagulation or by adsorption, a significant reduction of membrane fouling was observed in tests using two different types of ultrafiltration flat-sheet membranes in 20-h cross-flow filtration tests.     

Identification of biofoulant of membrane bioreactors in soluble microbial products

To reveal primary biofoulant in soluble microbial products (SMP) and/or soluble extracellular polymeric substances (EPS), after removal of sludge particles, activated sludge samples were subjected to microfiltration tests in a submerged MBR. Filtration resistance directly correlates with the saccharide concentration. Saccharides in wastewater from several sources contained uronic acids, which increased the filtration resistance. When the microfiltration test liquids contained saccharides over 80 mg l⁻¹, a gelatinous mass remained on the membrane surface after filtration and contained concentrations of saccharides and uronic acids 50 times higher than the original test liquid while only trace amounts of these substances were contained in the filtrate. The gelatinous mass contained high molecular weight substances of 10⁶-10⁸ Da, suggesting the presence of polysaccharides. However, molecules of this size were calculated to be much smaller than the pore size of the membrane. Ethylenediaminetetraacetic acid decreased filtration resistance, suggesting that polysaccharides containing uronic acid units could undergo intermolecular or intramolecular ionic cross-linking by polyvalent cations and form the gel, thus clogging the membrane pores as an actual biofoulant.