Membrane fouling characterisation in aerobic submerged membrane bioreactors

MEMBRANE FOULING CHARACTERISATION IN AEROBIC SUBMERGED MEMBRANE BIOREACTORS NG TZE CHIANG, ALBERT NATIONAL UNIVERSITY OF SINGAPORE 2010 MEMBRANE FOULING CHARACTERISATION IN AEROBIC SUBMERGED MEMBRANE BIOREACTORS NG TZE CHIANG, ALBERT (B. Eng (Hons), NUS) A THESIS SUBMITTED FOR THE DEGREE OF DOCTOR OF PHILOSOPHY DEPARTMENT OF CIVIL ENGINEERING NATIONAL UNIVERSITY OF SINGAPORE 2010 Acknowledgements ACKNOWLEDGEMENTS I would like to express my heartfelt gratitude to my supervisor, Dr. Ng How Yong for his intellectual guidance and invaluable support and advice throughout the course of this research project. Sincere thanks are extended to the members of the examination committee, as well as the external examiners for reviewing this thesis. I would also like to thank the staff of the Water Science and Technology Laboratory in the Division of Environmental Science and Engineering; Mr. Chandrasegaran, Ms. Lee Leng Leng, Ms. Tan Hwee Bee, and Ms. Tan Xiaolan, for their assistance in experimental support and with lab equipment. Contributions by final year student, Luo Chan are gratefully acknowledged. I wish to express my deepest thanks to my family, and my good friends in the lab, especially Ms. Hong Peiying, Ms. Huang Zhi, Ms. Jin Le, Mr. Ooi Wai Keong, Mr. Wong Sing Chuan for their support, and for making laboratory work less arduous than expected. Thanks for making my years in the lab so memorable! Finally, I have to thank Almighty God for blessing me with the strength and confidence to complete this research study, especially at times of immense difficulty. Membrane Fouling Characterisation in Aerobic Submerged Membrane Bioreactors Table of Contents TABLE OF CONTENTS Table of Contents i Summary vii Nomenclature x List of Tables xiii List of Figures xv Publications xix CHAPTER 1: INTRODUCTION 1.1 Background 1.2 Problem Statements 1.2.1 1.2.2 1.2.3 1.2.4 1.3 Mechanism of Fouling Development in MBRs operated at Different Flux Conditions Microstructure of Organic Fouling Layer associated with Membrane Fouling Macrostructure of Fouling Layer for Monitoring of Membrane Fouling in MBRs 10 Community Structure of Biofilms associated with Membrane Fouling 11 Research Objectives 12 CHAPTER 2: LITERATURE REVIEW 2.1 2.2 Membrane Bioreactors (MBRs) 15 2.1.1 MBR History, Reactor and Membrane Configurations 15 2.1.2 Critical and Sustainable Flux 16 Factors affecting Membrane Fouling 17 2.2.1 19 19 20 Membrane Material and Module related Parameters 2.2.1.1 Physical Characteristics 2.2.1.2 Chemical Characteristics Membrane Fouling Characterisation in Aerobic Submerged Membrane Bioreactors Page | i Table of Contents 2.2.2 2.2.3 2.3 Operating Condition related Parameters 2.2.2.1 Operating Flux and Hydraulic Retention Time (HRT) 2.2.2.2 Solids Retention Time (SRT) Biomass (Sludge) related Parameters 2.2.3.1 Mixed Liquor Suspended Solids (MLSS) Concentration 2.2.3.2 Relative Hydrophobicity (RH) 2.2.3.3 Extracellular Polymeric Substances (EPS) and Soluble Microbial Products (SMP) Concentrations 2.2.3.4 Microbial Community 22 22 24 25 25 27 29 35 Fouling Mechanism in MBRs 36 2.3.1 Constant Transmembrane Pressure (TMP) Operation 36 2.3.2 Constant Flux Operation 37 2.4 Biofilms 40 2.5 Biofilm Formation as a Developmental Process 41 2.6 Problems associated with Biofilms 43 2.7 Biofilm Structure 44 2.7.1 EPS 45 2.7.2 Quantifying Biofilm Structure 46 2.8 Macroscopic Characterisation of Membrane Fouling 50 2.9 Summary 51 CHAPTER 3: MATERIALS AND METHODS 3.1 Submerged Membrane Bioreactor (sMBR) Setup 53 3.2 Operating Conditions 56 3.3 Sampling Methods 59 3.3.1 Sampling Design 59 3.3.2 Membrane Sections 59 3.3.3 Liquid Samples 60 3.4 Analytical Methods 61 3.4.1 Membrane Surface Contact Angle Measurements 61 3.4.2 Mixed Liquor Suspended Solids (MLSS) and Mixed Liquor Volatile Solids (MLVSS) 61 Membrane Fouling Characterisation in Aerobic Submerged Membrane Bioreactors Page | ii Table of Contents 3.4.3 Molecular Weight (MW) Distribution 61 3.4.4 Sludge Relative Hydrophobicity 62 3.4.5 Sludge Surface Zeta Potential 62 3.4.6 Soluble Microbial Products (SMP) and Extracellular Polymeric Substances (EPS) 3.4.6.1 Extraction 3.4.6.2 Carbohydrate Concentration 3.4.6.3 Protein Concentration 63 63 64 64 3.4.7 Excitation-Emission Matrix (EEM) 65 3.4.8 Microscopic Observation of Fouling Layer 3.4.8.1 Fixation and Embedment 3.4.8.2 Fluorescent Staining 3.4.8.3 Confocal Laser Scanning Microscopy (CLSM) and Image Analysis 3.4.8.4 Scanning Electron Microscopy (SEM) 66 66 66 68 69 3.4.9 Macroscopic Observation of Fouling Layer 69 3.4.10 Molecular Biology Based Techniques for the Fingerprinting of the Microbial Community 3.4.10.1 Sample Collection 3.4.10.2 Total Community Deoxyribonucleic Acid (DNA) Extraction 3.4.10.3 Polymeric Chain Reaction (PCR) 3.4.10.4 Terminal Restriction Fragment Length Polymorphism (t-RFLP) 70 70 71 72 72 CHAPTER 4: ANALYSIS OF FOULING LAYER IN MBRS UNDER DIFFERENT OPERATING FLUX CONDITIONS 4.1 Introduction 74 4.2 Results and Discussions 76 4.2.1 76 76 Physico-Chemical Characterisation 4.2.1.1 Membrane Fouling Performance 4.2.1.2 Effect of Biomass Characteristics on Membrane Fouling: Mixed Liquor Suspended Solids (MLSS) Concentration, Sludge Relative Hydrophobicity (RH), and Sludge Zeta Potential 4.2.1.3 Effect of Soluble Microbial Products (SMP) and Extracellular Polymeric Substances (EPS) Concentrations on Membrane Fouling 4.2.1.4 Molecular Weight (MW) Distribution Profiles Membrane Fouling Characterisation in Aerobic Submerged Membrane Bioreactors 79 84 88 Page | iii Table of Contents 4.2.1.5 4.2.2 Excitation-Emission Matrices (EEM) 91 Micro-Structural Characterisation of Fouling Layer 4.2.2.1 Bio-Volume (BV) of Foulants 4.2.2.2 Porosity (P) of Foulants 93 94 99 4.3 Effect of Foulants and Fouling Parameters on Membrane Fouling 102 4.4 Summary 109 CHAPTER 5: ANALYSIS OF MEMBRANE FOULING IN MBRS UNDER DIFFERENT SOLIDS RETENTION TIMES 5.1 Introduction 110 5.2 Results and Discussions 112 5.2.1 112 112 5.2.2 Physico-Chemical Characterisation 5.2.1.1 Membrane Fouling Performance 5.2.1.2 Effect of Biomass Characteristics on Membrane Fouling: Mixed Liquor Suspended Solids (MLSS) Concentration, Sludge Relative Hydrophobicity (RH), and Sludge Zeta Potential 5.2.1.3 Effect of Soluble Microbial Products (SMP) and Extracellular Polymeric Substances (EPS) Concentrations on Membrane Fouling 5.2.1.4 Molecular Weight (MW) Distribution Profiles 5.2.1.5 Excitation-Emission Matrices (EEM) 120 123 Micro-Structural Characterisation of Fouling Layer 5.2.2.1 Bio-Volume (BV) of Foulants 5.2.2.2 Porosity (P) of Foulants 125 126 132 114 117 5.3 Effect of Foulants and Fouling Parameters on Membrane Fouling 137 5.4 Summary 142 CHAPTER 6: FOULING MECHANISM OF DIFFERENT MEMBRANE MATERIALS 6.1 Introduction Membrane Fouling Characterisation in Aerobic Submerged Membrane Bioreactors 143 Page | iv Table of Contents 6.2 Results and Discussions 145 6.2.1 145 145 6.2.2 Physico-Chemical Characterisation 6.2.1.1 Membrane Fouling Performance 6.2.1.2 Effect of Biomass Characteristics on Membrane Fouling: Mixed Liquor Suspended Solids (MLSS) Concentration, Sludge Relative Hydrophobicity (RH), and Sludge Zeta Potential 6.2.1.3 Effect of Soluble Microbial Products (SMP) and Extracellular Polymeric Substances (EPS) Concentrations on Membrane Fouling 6.2.1.4 Molecular Weight (MW) Distribution Profiles 6.2.1.5 Excitation-Emission Matrices (EEM) 153 155 Micro-Structural Characterisation of Fouling Layer 6.2.2.1 Bio-Volume (BV) of Foulants 6.2.2.2 Porosity (P) of Foulants 157 158 170 147 151 6.3 Effect of Foulants and Fouling Parameters on Membrane Fouling 175 6.4 Summary 182 CHAPTER 7: ECOLOGICAL AND RAPID CHARACTERISATION OF MEMBRANE FOULING IN MBRS 7.1 Introduction 183 7.2 Results and Discussions 185 7.2.1 Light Microscopy 185 7.2.2 Scanning Electron Microscopy (SEM) 187 7.2.3 Confocal Laser Scanning Microscopy (CLSM) 190 7.2.4 Ecological Characterisation of Microbial Community 191 7.2.5 Rapid Characterisation of Membrane Fouling in MBRs 208 7.2.5.1 7.2.5.2 7.3 Macroscopic Imaging of Membrane Surface Rapid Characterisation of Microbial Community Summary Membrane Fouling Characterisation in Aerobic Submerged Membrane Bioreactors 208 210 213 Page | v Table of Contents CHAPTER 8: CONCLUSIONS AND RECOMMENDATIONS 215 8.1 215 Conclusions 8.1.1 Analysis of Fouling Layer in MBRs under Different Operating Flux Conditions 215 Analysis of Membrane Fouling in MBRs under Different Solids Retention Times 216 8.1.3 Fouling Mechanisms of Different Membrane Materials 217 8.1.4 Ecological and Rapid Characterisation of Membrane Fouling in MBRs 219 8.1.2 8.2 Recommendations 8.2.1 220 Examination of Membrane Fouling using Appropriate Techniques 220 8.2.2 Fouling Control Strategies 221 8.2.3 Identification of Ecological Niches within Fouling Layer 222 REFERENCES Membrane Fouling Characterisation in Aerobic Submerged Membrane Bioreactors 224 Page | vi Summary SUMMARY The presence of an organic fouling layer in membrane bioreactors (MBRs) can compromise membrane integrity through the biodegradation of membrane material and lead to the ultimate failure of the membrane process. To date, many studies have been conducted to elucidate and assess the effects that a myriad of parameters have on membrane fouling in MBRs. Conflicting results have been attained between research groups. Most studies conducted thus far focused on the effect of operating parameters on fouling profiles; not on the fouling mechanism. A serious flaw in the studies claiming to focus on membrane fouling mechanisms is the use of easily quantifiable parameters in the bulk solution. This research study aimed to reveal and distinguish fouling mechanisms under different operating conditions by studying the foulants on membrane surfaces. Fouling characteristics of aerobic submerged MBRs were analysed under different flux conditions. Micro-structural analyses of the foulants on the membrane surfaces showed that the dominant foulants were different under different flux conditions. Membrane fouling occurred through a biofilm dominated process under lower flux conditions, but the mechanism shifted towards a non-biofilm, bio-organic fouling process as the flux was increased. In spite of the differences in fouling mechanisms, it was found that the protein fraction on the membrane surface had the greatest impact in the rise of transmembrane pressure. Membrane Fouling Characterisation in Aerobic Submerged Membrane Bioreactors Page | vii References Germain E., and Stephenson T. (2005) Biomass Characteristics, Aeration and Oxygen Transfer in Membrane Bioreactors: their Interrelations explained by a review of Aerobic Biological Processes. Reviews in Environmental Science and Bio/Technology, 4, pp. 223 – 233. Ghayeni S.B.S., Beatson P.J., Schneider R.P., and Fane A.G. (1998) Adhesion of Waste Water Bacteria to Reverse Osmosis Membranes. Journal of Membrane Science, 138, pp. 29 – 42. Gilbert P., Evans D.J., Evans E., Duguid I.G., and Brown M.R. 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Membrane Fouling Characterisation in Aerobic Submerged Membrane Bioreactors Page | 244 [...]... fundamental fouling issue in MBRs, yet bio-organic fouling could be as important as well In addition, the effects of different operating conditions on membrane biofouling are also not well-understood Membrane Fouling Characterisation in Aerobic Submerged Membrane Bioreactors Page | 8 Chapter 1 1.2.2 Microstructure Introduction of Organic Fouling Layer associated with Membrane Fouling Despite being commercially... 2000) Membrane Fouling Characterisation in Aerobic Submerged Membrane Bioreactors Page | 4 Chapter 1 Introduction The formation of a fouling layer on membrane surfaces is responsible for a number of operational inefficiencies in MBR systems Fouling layers of 10 to 100 µm thickness have been reported to create a considerable increase in membrane resistance, which resulted in a corresponding decline in. .. method of determining membrane fouling mechanism would be to identify the compounds on the membrane surface, and determine the effect each constituent has on membrane fouling As such, the mechanism of membrane fouling may be better studied in terms of the foulants within the fouling layer in an in- situ condition Membrane biofouling mechanisms are comparatively more well-known Typical biofouling mechanisms... process is constrained by deposition of unwanted materials on the membrane surface, or membrane fouling Membrane fouling is a severe operational problem in MBRs and has been shown to contribute to a loss in membrane productivity through reductions in permeate fluxes, Membrane Fouling Characterisation in Aerobic Submerged Membrane Bioreactors Page | 3 Chapter 1 Introduction increases in differential pressure... for biofouling A better understanding of the different nature of the structure of the fouling layer in relation to the operating flux, solids retention tine (SRT), and membrane material may explain the effect bulk parameters have on membrane fouling and aid in developing more accurate equations to describe and model membrane fouling in MBRs 1.2.3 Macrostructure of Fouling Layer for Monitoring of Membrane. .. Such areas promote Membrane Fouling Characterisation in Aerobic Submerged Membrane Bioreactors Page | 10 Chapter 1 Introduction membrane fouling to a greater extent even though the observed TMP may be low, thereby lulling MBR operators into a false sense of security A simple surface characterisation technique is thus needed Studies involving characterisation of the fouling layer on membrane surfaces... microbial products SMPc SMP-carbohydrate SMPp SMP-protein SUVA specific ultra-violet absorption t-RFLP terminal restriction fragment length polymorphism Membrane Fouling Characterisation in Aerobic Submerged Membrane Bioreactors Page | xi Abbreviations TMP transmembrane pressure UF ultrafiltration Membrane Fouling Characterisation in Aerobic Submerged Membrane Bioreactors Page | xii List of Tables LIST OF TABLES... that membrane fouling mechanism shifted from a biofilm initiated process on PO membranes to a bio-organic dominated process on PES membranes under sub-critical flux conditions The fouling mechanisms were similar on both membrane materials at higher flux conditions Physico-chemical characterisation was unable to explain the differences in membrane fouling of the contrasting membrane materials indicating... A serious flaw in studies focusing on membrane fouling mechanisms is the use of easily quantifiable parameters in the bulk solution Using various biomass characteristics to reveal the fouling mechanism has commonly been used but may not represent the actual foulants found on the membrane surface The difference in soluble Membrane Fouling Characterisation in Aerobic Submerged Membrane Bioreactors Page... revealed a distinct trend in fouling mechanisms based on differences in flux conditions Such analytical methods have Membrane Fouling Characterisation in Aerobic Submerged Membrane Bioreactors Page | viii Summary shown to be effective in being able to accurately describe membrane fouling mechanisms Thus, appropriate and more effective fouling control strategies may be developed based in the results published . MEMBRANE FOULING CHARACTERISATION IN AEROBIC SUBMERGED MEMBRANE BIOREACTORS NG TZE CHIANG, ALBERT NATIONAL UNIVERSITY OF SINGAPORE 2010 MEMBRANE FOULING CHARACTERISATION. the rise of transmembrane pressure. Summary Membrane Fouling Characterisation in Aerobic Submerged Membrane Bioreactors Page | viii Fouling characteristics of aerobic submerged MBRs were. Membrane Fouling Characterisation in Aerobic Submerged Membrane Bioreactors Page | v 6.2 Results and Discussions 145 6.2.1 Physico-Chemical Characterisation 145 6.2.1.1 Membrane Fouling