Early fouling warning is important for the economical operation of membrane separation systems. In parallel multi-channel flow systems, flow re-distribution between channels due to fouling is often associated with maloperation. In the current research we use low magnetic field NMR to monitor multi-fiber hollow fiber membrane modules undergoing a fouling-cleaning cycle and show that rapid detection of fouling is possible by detecting the loss of signal coherence associated with flow re-distribution within the 401 hollow fiber membrane module. This effect is demonstrated to be both reproducible, and reversible via membrane cleaning. The results demonstrate a strong correlation between the coherence signal magnitude and the number of fibers fouled. This may be used in practice for high sensitivity early warning, and to monitor the efficiency of cleaning. This approach may also be particularly useful in the case of detecting residual fouling after cleaning, evidenced in this research by significant flow re-distribution between the before fouling and after cleaning signal coherence.

In this study non-invasive low field magnetic resonance imaging (MRI) technology was used to monitor fouling induced changes in fiber-by-fiber hydrodynamics inside a multi-fiber hollow fiber membrane module containing 401 fibers. Using structural and velocity images the fouling evolution of these membrane modules were shown to exhibit distinct trends in fiber-by-fiber volumetric flow, with increasing fouling causing a decrease in the number of flow active fibers. This study shows that the fouling rate is not evenly distributed over the parallel fibers, which results in a broadening of the fiber to fiber flowrate distribution. During cleaning, this distribution is initially broadened further, as relatively clean fibers are cleaned more rapidly compared to clogged fibers. By tracking the volumetric flow rate of individual fibers inside the modules during the fouling-cleaning cycle it was possible to observe a fouling memory-like effect with residual fouling occurring preferentially at the outer edge of the fiber bundle during repeated fouling-cleaning cycle. These results demonstrate the ability of MRI velocity imaging to quantitatively monitor these effects which are important when testing the effectiveness of cleaning protocols due to the long term effect that residual fouling and memory-like effect may have on the operation of membrane modules.

The application of membrane technology for water treatment and reuse is hampered by the development of a microbial biofilm. Biofilm growth in micro-and ultrafiltration (MF/UF) membrane modules, on both the membrane surface and feed spacer, can form a secondary membrane and exert resistance to permeation and crossflow, increasing energy demand and decreasing permeate quantity and quality. In recent years, exhaustive efforts were made to understand the chemical, structural and hydraulic characteristics of membrane biofilms. In this review, we critically assess which specific structural features of membrane biofilms exert resistance to forced water passage in MF/UF membranes systems applied to water and wastewater treatment, and how biofilm physical structure can be engineered by process operation to impose less hydraulic resistance (“below-the-pain threshold”). Counter-intuitively, biofilms with greater thickness do not always cause a higher hydraulic resistance than thinner biofilms. Dense biofilms, however, had consistently higher hydraulic resistances compared to less dense biofilms. The mechanism by which density exerts hydraulic resistance is reported in the literature to be dependant on the biofilms’ internal packing structure and EPS chemical composition (e.g., porosity, polymer concentration). Current reports of internal porosity in membrane biofilms are not supported by adequate experimental evidence or by a reliable methodology, limiting a unified understanding of biofilm internal structure. Identifying the dependency of hydraulic resistance on biofilm density invites efforts to control the hydraulic resistance of membrane biofilms by engineering internal biofilm structure. Regulation of biofilm internal structure is possible by alteration of key determinants such as feed water nutrient composition/concentration, hydraulic shear stress and resistance and can engineer biofilm structural development to decrease density and therein hydraulic resistance. Future efforts should seek to determine the extent to which the concept of “biofilm engineering” can be extended to other biofilm parameters such as mechanical stability and the implication for biofilm control/removal in engineered water systems (e.g., pipelines and/or, cooling towers) susceptible to biofouling.

A novel magnetic resonance measurement (MRM) protocol for non-invasive monitoring of fouling in spiral wound reverse osmosis (SWRO) membrane modules is demonstrated. Sodium alginate was used to progressively foul a commercial SWRO membrane at industrially relevant operating conditions in a circulating flow loop. The MRM protocol showcased the following: (i) earlier, more sensitive detection and quantification of fouling in the membrane module compared to feed-channel pressure drop. This was achieved using appropriate detection of the total nuclear magnetic resonance (NMR) signal. (ii) 2D cross-sectional imaging of the location of the accumulated foulant material; this was preferentially located adjacent to the membrane spacer sheet nodes, which was subsequently confirmed by a module autopsy. This image contrast, which could also readily differentiate the membrane, feed spacer and permeate spacer regions, was realised based on differences in the NMR relaxation parameter, T_2,eff. (iii) High frequency acquisition of 2D cross-sectional velocity images of the module revealing very localised flow channelling in response to gradual foulant accumulation which impacted significantly on the flow pattern within the central permeate tube. Collectively this NMR/MRI measurement protocol provides a powerful analysis tool for the evolution of fouling in such complex modules, thus ultimately enabling more informed module design.

Forward osmosis (FO) and reverse osmosis (RO) membrane processes differ in their driving forces: osmotic pressure versus hydraulic pressure. Concentration polarization (CP) can adversely affect both performance and lifetime in such membrane systems. In order to mitigate against CP, the extent and severity of it need to be predicted more accurately through advanced online monitoring methodologies. Whilst a variety of monitoring techniques have been used to study the CP mechanism, there is still a pressing need to develop and apply non-invasive, in situ techniques able to produce quantitative, spatially resolved measurements of heterogeneous solute concentration in, and adjacent to, the membrane assembly as caused by the CP mechanism. To this end, ²³Na magnetic resonance imaging (MRI) is used to image the sodium ion concentration within, and near to, both FO and RO composite membranes for the first time; this is also coupled with ¹H MRI mapping of the corresponding water distribution. As such, it is possible to directly image salt accumulation due to CP processes during desalination. This was consistent with literature expectations and serves to confirm the suitability of ²³Na MRI as a novel non-invasive technique for CP studies.

Magnetic Resonance Imaging (MRI) velocimetry was applied to study non-invasively the water flow field inside a spiral-wound desalination membrane module (diameter: 2.5 in.; length: 18.5 in.), located in a pressure vessel, at typical practice operational conditions as a function of alginate fouling, simulating extracellular polymeric substances (EPS). Cross-sectional velocity images were acquired at an in-plane spatial resolution of 0.137 mm at multiple locations along the length of the reverse osmosis module and were acquired as a function of alginate concentration. At a total system alginate concentration of 3.25 mg/l, significant changes in the cross-sectional velocity map were observed near the module inlet due to alginate fouling, with limited changes observed in the middle and outlet regions of the module. When the total system alginate concentration was increased to 75 mg/l, it caused the module brine seal to fail resulting in significant local water flow by-passing the membrane module. This was clearly discernible in this opaque membrane system using MRI and resulting in dramatic changes in fluid velocity distribution through the membrane module. These observations of significant flow field heterogeneity as fouling develops are consistent with ‘irreversible’ fouling effects noted frequently in practice by the water treatment industry.

Fouling of spiral-wound reverse osmosis (SWRO) membrane systems is a pervasive problem. Here we demonstrate that a mobile, low cost magnetic resonance imaging (MRI) apparatus operating at the earth’s magnetic field (low magnetic field, LF) can non-invasively (i) image the inside of a SWRO membrane system with glass fiber outside casing in a pressure vessel during cross flow operation and can (ii) detect the location of foulant, in this study sodium alginate. LF-MRI images of the module were successfully acquired in less than eight minutes using a spin-echo protocol, the internal structure of the modules was clearly evident and images compared well with high resolution MRIs obtained using a large-sized, costly high magnetic field superconducting MRI system. By parameter optimisation (specifically the echo time employed) it was possible to differentiate flowing and stagnant fluid in the clean and fouled membrane systems, and to determine the presence of alginate foulant on the feed-side of the fouled SWRO membrane system. This study motivates further investigation of the sensitivity of LF-MRI and the development of bespoke low cost LF-MRI hardware for the monitoring of industrial SWRO membrane installations.

Membrane systems are commonly used in the water industry to produce potable water and for advanced wastewater treatment. One of the major drawbacks of membrane systems is biofilm formation (biofouling), which results in an unacceptable decline in membrane performance. Three novel in situ biofouling characterization techniques were assessed: (i) optical coherence tomography (OCT), (ii) planar optodes, and (iii) nuclear magnetic resonance (NMR). The first two techniques were assessed using a biofilm grown on the surface of nanofiltration (NF) membranes using a transparent membrane fouling simulator that accurately simulates spiral wound modules, modified for in situ biofilm imaging. For the NMR study, a spiral wound reverse osmosis membrane module was used. Results show that these techniques can provide information to reconstruct the biofilm accurately, either with 2-D (OCT, planar optodes and NMR), or 3-D (OCT and NMR) scans. These non-destructive tools can elucidate the interaction of hydrodynamics and mass transport on biofilm accumulation in membrane systems. Oxygen distribution in the biofilm can be mapped and linked to water flow and substrate characteristics; insights on the effect of crossflow velocity, flow stagnation, and feed spacer presence can be obtained, and in situ information on biofilm structure, thickness, and spatial distribution can be quantitatively assessed. The combination of these novel non-destructive in situ biofilm characterization techniques can provide real-time observation of biofilm formation at the mesoscale. The information obtained with these tools could potentially be used for further improvement in the design of membrane systems and operational parameters to reduce impact of biofouling on membrane performance.