The main obstacle for wider use of membrane bioreactors (MBRs) for wastewater treatment is membrane fouling (i.e., deterioration of membrane permeability),which increases operating costs. For more efficient control of membrane fouling in MBRs, an understanding of the mechanisms of membrane fouling is important. However, there is a lack of information on membrane fouling in MBRs, especially information on features of components that are responsible for the fouling. We conducted a pilot-scale experiment using real municipal wastewater with three identical MBRs under different operating conditions. The results obtained in this study suggested that the food-microorganisms ratio (F/M) and membrane filtration flux were the important operating parameters that significantly influenced membrane fouling in MBRs. Neither concentrations of dissolved organic matter in the reactors nor viscosity of mixed liquor, which have been thought to have influences on fouling in MBRs, showed clear relationships with membrane fouling in this study. Organic substances that had caused the membrane fouling were desorbed from fouled membranes of the MBRs at the termination of the operation and were subjected to Fourier transform infrared (FTIR) and 13C nuclear magnetic resonance (NMR) analyses. These analyses revealed that the nature of the membrane foulant changes depending on F/M. It was shown that high F/M would make the foulant more proteinaceous. Carbohydrates were dominant in membrane foulants in this study, while features of humic substances were not apparent.
The elimination of six acidic pharmaceuticals (clofibric acid, diclofenac, ibuprofen, ketoprofen, mefenamic acid, and naproxen) in a real wastewater treatment plant (WWTP) using an activated sludge system and membrane bioreactors (MBRs) was investigated by using a gas chromatography/mass spectrometry (GC/MS) system for measurement of the compounds. Limited information is available for some of the tested pharmaceuticals at present. Solid retention times (SRTs) of the WWTP and the two MBRs were 7, 15, and 65 days, respectively. The elimination rates varied from compound to compound. The MBRs exhibited greater elimination rates for the examined pharmaceuticals than did the real plant. Dependency of the elimination rates of the pharmaceuticals on SRTs was obvious; the MBR operated with a longer SRT of 65 days clearly showed better performance than did the MBR with a shorter SRT of 15 days. The difference between the two MBRs was particularly significant in terms of elimination of ketoprofen and diclofenac. Measurements of the amounts of adsorbed pharmaceuticals on the sludge and aerobic batch elimination experiments were carried out to investigate the elimination pathways of the pharmaceuticals. Results of the batch elimination tests revealed that the sludges in the MBRs had large specific sorption capacities mainly due to their large specific surface areas. Despite the sorption capacities of sludges, the main mechanism of elimination of the pharmaceuticals in the investigated processes was found to be biodegradation. Biodegradation of diclofenac, which has been believed to be refractory to biodegradation, seemed to occur very slowly.
Control of membrane fouling is important for more efficient use of membranes in water treatment. Control of physically irreversible fouling, which is defined as fouling that requires chemical cleaning to be cancelled, is particularly important for reduction of operation cost in a membrane process. In this study, a long-term filtration experiment using three different types of MF and UF membranes was carried out at an existing water purification plant, and the evolution of physically irreversible fouling was investigated. The experimental results demonstrated that the extent of physically irreversible fouling differed significantly depending on the membrane type. Cleaning of the fouled membranes with various chemical reagents demonstrated that organic matter was mainly responsible for physically irreversible fouling. Organic matter that had caused physically irreversible fouling in the long-term operation was desorbed from the fouled membranes and was subjected to Fourier transform infrared and 13C nuclear magnetic resonance analyses. These analyses revealed that carbohydrates were dominant in the membrane foulant regardless of the type of membrane. Based on measurements of molecular weight distribution of organic matter in the feedwater and the permeates from the membranes, a two-step fouling mechanism is proposed to explain the dominance of carbohydrates in the foulant: hydrophobic (humic-like) components with small molecular weight are first adsorbed on the membrane and, consequently, narrow the size of micro-pores of membranes, and then hydrophilic (carbohydrate-like) compounds with larger molecular weight plug the narrowed pores or the hydrophilic compounds are adsorbed onto the membrane surface conditioned by the hydrophobic components.
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