University of Wollongong Research Online Removal of trace organic contaminants by integrated membrane processes for indirect potable water reuse applications Abdulhakeem Alturki University of Wollongong School of Civil, Mining and Environmental Engineering Removal of Trace Organic Contaminants by Integrated Membrane Processes for Indirect Potable Water Reuse Applications Abdulhakeem Alturki This thesis is presented as part of the requirements for the award of the Degree of the Doctor of Philosophy University of Wollongong January, 2013 CERTIFICATION i ABSTRACT The occurrence of trace organic contaminants (TrOCs), both from anthropogenic and naturally occurring origins, in the aquatic environment is of concern from environmental and human health protection perspective Many of these TrOCs are ubiquitous in domestic wastewater and advanced treatment processes are required to ensure their removal to a safe level if the reclaimed water is intended for indirect potable water recycling applications This thesis work investigated the removal of TrOCs by three integrated membrane processes for indirect potable water recycling applications The results reported in this thesis indicate that a combination of membrane bioreactor (MBR) with nanofiltration (NF) or reverse osmosis (RO) membrane filtration can complement each other very well to efficiently remove a wide range of TrOCs Forward osmosis (FO) is an emerging treatment technology and results reported here also showed some promising aspects of this process for the removal of TrOCs The innovative combination of FO in combination with MBR in the form of osmotic membrane bioreactor (OMBR) for the removal of TrOCs was also investigated in this thesis work The results are preliminary but demonstrate the potential of this approach as a low energy process for the production of high quality treated effluent, particularly when discharging into the ocean (i.e seawater is readily available as the draw solution) The removal of TrOCs by a hybrid treatment process incorporating an MBR with NF/RO filtration was investigated Using a laboratory scale MBR system and a cross-flow NF/RO system, experiments were conducted with 40 organic compounds representing the major groups of TrOCs found in wastewater The results suggest that the MBR system could effectively remove hydrophobic and biodegradable trace organic compounds, while the remaining trace organic compounds (mostly hydrophilic) were effectively removed by the NF/RO membranes The combination of MBR and a low pressure RO membrane resulted in more than 95% removal (or removal to below the limits of analytical detection), for all the compounds investigated in this study Results reported in this research component also suggest that fouling mitigation of the NF/RO membranes can be adequately controlled The rejection of TrOCs by an osmotically driven membrane filtration process was also investigated using a set of 40 compounds Their rejection by an FO membrane ii specifically designed for the osmotically driven process and a tight NF membrane was systematically investigated and compared under three different operating modes, namely forward osmosis (FO), pressure retarded osmosis (PRO), and reverse osmosis (RO) The results revealed that the FO membrane had a considerably higher water flux than the NF membrane when operated in either the FO or PRO modes However, the NF membrane consistently rejected the contaminants better than the FO membrane In the RO mode, electrostatic interactions played a dominant role in governing the rejection of charged compounds, whereas in the FO and PRO modes, their rejection was governed by both electrostatic interaction and size exclusion On the other hand, the rejection of neutral compounds was dominated by size exclusion, with rejection increasing with the molecular weight of the component The PRO mode resulted in a higher water flux but a notably lower rejection of TrOCs than with the FO mode It is also noteworthy that the rejection of neutral compounds in the FO mode was higher than in the RO mode This behavior could be attributed to the retarded forward diffusion occurring in the FO mode The removal of TrOCs using an innovative OMBR system was also investigated Following an initial gradual decline, a stable permeate flux value was obtained after approximately four days of continuous operation, although the biological activity of the OMBR system continued to deteriorate, possibly due to the build-up of salinity in the reactor The OMBR mostly removed the large molecular weight trace organic compounds by above 80% and was possibly governed by the interplay between the physical separation of the FO membrane and biodegradation Whereas, the removal efficiency of smaller trace organic compounds by OMBR was scattered and appeared to depend mostly on biological degradation iii ACKNOWLEDGEMENTS This thesis has proven to be an amazing challenge in that it has allowed me to meet and work with people from different countries, which has made my study much more enjoyable Throughout this period of study I have received enormous support and encouragement and now that it has ended it will be the start of a new research life I am very grateful to my supervisors, Associate Prof Long Duc Nghiem and Prof Will Price, for their guidance, patience, and for having me in their research world because I have gained knowledge and experience which I would not have received without their insight and support I would also like to thank the Ministry of Higher Education in Saudi Arabia and the Saudi Arabian Cultural Mission in Australia for providing me a PhD scholarship with generous financial support for me and my family I would like to thank my parents, both of whom are the reason for my experiences in this life, and to my brothers and sisters for their moral support and infinite love during the difficult times, while always pushing me to succeed with my studies I would also like to thank our collaborators, Dr Stuart Khan and Dr James McDonald from the Water Research Centre at the University of New South Wales for their continuous support for my research It has also been a great experience working and getting guidance and assistance from Dr Faisal Hai, it is greatly appreciated The Hydration Technology Innovations and Dow Film Tec (Minneapolis, MN), Koch Membrane Systems (San Diego, CA), and Zenon Environment (Toronto, Cananda) are also thanked for providing membrane samples for this project My soul partner, my wife, the real supporter during my ordeal or sickness is thankful for every moment spent with me, or with our children Farah and Ali, both of whom are the pleasant colours of our life iv Special thanks to our staff and students at the Environmental Engineering and Strategic Water Infrastructure Laboratories, in particular Adam Kiss, Nichanan Tadkaew, Luong Nguyen, Farhat Saeed, Rajab Abousnina, and Le Kha Tu for all the support and exchange of knowledge in a very friendly environment The technical staff of the Engineering Faculty, Bob Rowlan and Frank Crabtree, are greatly thanked for their constant hard work and the pleasant manner in which they provided solutions to the many problems that surfaced during my research Finally, thanks to every friend or family member who has not been mentioned here, but who have all contributed to making my life easier, and more enjoyable and valuable v TABLE OF CONTENTS CERTIFICATION i ABSTRACT ii TABLE OF CONTENTS vi LIST OF FIGURES ix LIST OF TABLES xiii LIST OF ABBREVIATIONS xiv Chapter 1: 1.1 Introduction Back ground 1.1.1 Trace organic contaminants in the environment 1.1.2 Effects of trace organic contaminants 1.1.3 The removal of trace organic contaminants by advanced treatment 1.2 Objectives of the Research 1.3 Thesis outline Chapter 2: Literature review 2.1 Introduction 2.2 Types of trace organic contaminants 2.3 Occurrence of trace organic contaminants in the aquatic environment 11 2.4 Effects of trace organic contaminants 13 2.4.1 Effects on aquatic organisms .13 2.4.2 Effects on human health and wildlife 15 2.5 Membrane technology .16 2.5.1 High pressure membrane filtration .16 2.5.2 Trace organic contaminants removal by MBR .21 2.5.3 Forward osmosis 30 2.6 Other advanced treatment processes 47 2.6.1 Activated carbon adsorption 47 2.6.2 Advanced oxidation processes .49 2.7 Conclusions .50 Chapter 3: 3.1 Materials and Methods .52 Introduction .52 vi 3.2 Model wastewater 52 3.2.1 MBR-NF/RO wastewater 52 3.2.2 FO wastewater .52 3.2.3 OMBR wastewater 53 3.3 Membranes and membrane modules 53 3.3.1 Ultrafiltration membrane modules for the MBR system .53 3.3.2 Nanofiltration and reverse osmosis (NF/RO) membranes .54 3.3.3 Forward osmosis (FO) membrane 55 3.4 Laboratory-scale set-ups 55 3.4.1 Laboratory-scale membrane bioreactor (MBR) 56 3.4.2 Pressure driven membrane filtration system 56 3.4.3 Osmotically driven membrane system 57 3.4.4 Osmotic bioreactor (OMBR) set-up .60 3.5 Experimental protocols 63 3.5.1 Hybrid MBR-NF/RO system .63 3.5.2 Osmotically driven membrane experimental protocol 64 3.5.3 Osmotic bioreactor experimental protocol 65 3.6 Membrane characterization techniques 67 3.6.1 Determination of membrane active layer transport properties .67 3.6.2 Contact angle measurement 67 3.6.3 Zeta potential measurement 68 3.7 Model trace organic contaminants 68 3.8 Analytical techniques 81 3.8.1 Analysis of basic water parameters 81 3.8.2 Sludge strength and characteristics .81 3.8.3 Trace organic component analysis .82 Chapter 4: The combination of MBR and NF/RO process for trace organics removal 85 4.1 Introduction .85 4.2 Materials and methods .87 4.2.1 Model trace organic contaminants 88 4.3 Results and discussion .90 4.3.1 Effects of trace organics on basic MBR performance 90 vii References 65 66 67 68 69 70 71 72 73 74 75 76 77 78 79 80 McGinnis, R.L and M Elimelech, Energy requirements of ammonia-carbon dioxide forward osmosis desalination 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PUBLICATIONS Journal papers Alturki, A., J McDonald, S.J Khan, F.I Hai, W.E Price, and L.D Nghiem, Performance of a novel osmotic membrane bioreactor (OMBR) system: Flux stability and removal of trace organics Bioresource Technology, 2012 113: p 201-206 Alturki, A.A., N Tadkaew, J.A McDonald, S.J Khan, W.E Price, and L.D Nghiem, Combining MBR and NF/RO membrane filtration for the removal of trace organics in indirect potable water reuse applications Journal of Membrane Science, 2010 365(1-2): p 206-215 Vogel, D., A Simon, A.A Alturki, B Bilitewski, W.E Price, and L.D Nghiem, Effects of fouling and scaling on the retention of trace organic contaminants by a nanofiltration membrane: The role of cake-enhanced concentration polarisation Separation and Purification Technology, 2010 73(2): p 256-263 Alturki, A., J McDonald, S.J Khan, W.E Price, L.D Nghiem, and Menachem Elimelech, Removal of trace organic contaminants by the forward osmosis process Separation and Purification Technology, 2013 103(0): p 258-266 Conference papers and presentations Alturki, A., N Tadkaew, J McDonald, S.J Khan, W.E Price, and L.D Nghiem, Removal of trace organic contaminants by membrane bioreactor and nanofiltration/reverse osmosis: a comparison study Proceedings of the Environmental Research Event, 2010, Rockhampton,CQ University Alturki, A., J McDonald, S.J Khan, W.E Price, and L.D Nghiem, Rejection of steroid hormones by forward osmosis process Membrane Society of Australasia Symposium, 2011, Glenelg, South Australia 153 ... 1.1.1 Trace organic contaminants in the environment 1.1.2 Effects of trace organic contaminants 1.1.3 The removal of trace organic contaminants by advanced treatment 1.2 Objectives of. .. Effects of trace organics on basic MBR performance 90 vii 4.3.2 Removal of trace organics by MBR .92 4.3.3 Removal of trace organics by a combined MBR-NF/RO system 93 4.3.4 Performance of. .. Introduction 2.2 Types of trace organic contaminants 2.3 Occurrence of trace organic contaminants in the aquatic environment 11 2.4 Effects of trace organic contaminants 13 2.4.1