Periodic chemical cleaning with urea: disintegration of biofilms and reduction of key biofilm-forming bacteria from reverse osmosis membranes.

Biofouling is one of the major factors causing decline in membrane performance in reverse osmosis (RO) plants, and perhaps the biggest hurdle of membrane technology. Chemical cleaning is periodically carried out at RO membrane installations aiming to restore membrane performance. Typical cleaning agents used in the water treatment industry include sodium hydroxide (NaOH) and hydrochloric acid (HCl) in sequence. Rapid biofilm regrowth and related membrane performance decline after conventional chemical cleaning is a routinely observed phenomenon due to the inefficient removal of biomass from membrane modules. Since extracellular polymeric substances (EPS) make up the strongest and predominant structural framework of biofilms, disintegration of the EPS matrix should be the main target for enhanced biomass removal. Previously, we demonstrated at lab-scale the use of concentrated urea as a chemical cleaning agent for RO membrane systems. The protein denaturation property of urea was exploited to solubilize the proteinaceous foulants, weakening the EPS layer, resulting in enhanced biomass solubilization and removal from RO membrane systems. In this work, we investigated the impact of repeated chemical cleaning cycles with urea/HCl as well as NaOH/HCl on biomass removal and the potential adaptation of the biofilm microbial community. Chemical cleaning with urea/HCl was consistently more effective than NaOH/HCl cleaning over 6 cleaning and regrowth cycles. At the end of the 6 cleaning cycles, the percent reduction was 35% and 41% in feed channel pressure drop, 50% and 70% in total organic carbon, 30% and 40% in EPS proteins, and 40% and 66% in the peak intensities of protein-like matter, after NaOH/HCl cleaning and Urea/HCl cleaning, respectively. 16S ribosomal RNA (rRNA) gene sequencing of the biofilm microbial community revealed that urea cleaning does not select for key biofouling families such as Sphingomonadaceae and Xanthomonadaceae that are known to survive conventional chemical cleaning and produce adhesive EPS. This study reaffirmed that urea possesses all the desirable properties of a chemical cleaning agent, i.e., it dissolves the existing fouling layer, delays fresh fouling accumulation by inhibiting the production of a more viscous EPS, does not cause damage to the membranes, is chemically stable, and environmentally friendly as it can be recycled for cleaning.

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.

Effect of water temperature on biofouling development in reverse osmosis membrane systems.

Understanding the factors that determine the spatial and temporal biofilm development is a key to formulate effective control strategies in reverse osmosis membrane systems for desalination and wastewater reuse. In this study, biofilm development was investigated at different water temperatures (10, 20, and 30 °C) inside a membrane fouling simulator (MFS) flow cell. The MFS studies were done at the same crossflow velocity with the same type of membrane and spacer materials, and the same feed water type and nutrient concentration, differing only in water temperature. Spatially resolved biofilm parameters such as oxygen decrease rate, biovolume, biofilm spatial distribution, thickness and composition were measured using in-situ imaging techniques. Pressure drop (PD) increase in time was used as a benchmark as to when to stop the experiments. Biofilm measurements were performed daily, and experiments were stopped once the average PD increased to 40 mbar/cm. The results of the biofouling study showed that with increasing feed water temperature (i) the biofilm activity developed faster, (ii) the pressure drop increased faster, while (iii) the biofilm thickness decreased. At an average pressure drop increase of 40 mbar/cm over the MFS for the different feed water temperatures, different biofilm activities, structures, and quantities were found, indicating that diagnosis of biofouling of membranes operated at different or varying (seasonal) feed water temperatures may be challenging. Membrane installations with a high temperature feed water are more susceptible to biofouling than installations fed with low temperature feed water.

Early non-destructive biofouling detection and spatial distribution: Application of oxygen sensing optodes.

Biofouling is a serious problem in reverse osmosis/nanofiltration (RO/NF) applications, reducing membrane performance. Early detection of biofouling plays an essential role in an adequate anti-biofouling strategy. Presently, fouling of membrane filtration systems is mainly determined by measuring changes in pressure drop, which is not exclusively linked to biofouling. Non-destructive imaging of oxygen concentrations (i) is specific for biological activity of biofilms and (ii) may enable earlier detection of biofilm accumulation than pressure drop. The objective of this study was to test whether transparent luminescent planar O2 optodes, in combination with a simple imaging system, can be used for early non-destructive biofouling detection. This biofouling detection is done by mapping the two-dimensional distribution of O2 concentrations and O2 decrease rates inside a membrane fouling simulator (MFS). Results show that at an early stage, biofouling development was detected by the oxygen sensing optodes while no significant increase in pressure drop was yet observed. Additionally, optodes could detect spatial heterogeneities in biofouling distribution at a micro scale. Biofilm development started mainly at the feed spacer crossings. The spatial and quantitative information on biological activity will lead to better understanding of the biofouling processes, contributing to the development of more effective biofouling control strategies.