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Electropermutation Assisted by Ion-Exchange Textile - Removal of Nitrate from Drinking Water by Carl-Ola Danielsson Department of Mechanics

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Electropermutation Assisted by Ion-Exchange Textile - Removal of Nitrate from Drinking Water by Carl-Ola Danielsson Department of Mechanics Electropermutation Assisted by Ion-Exchange Textile - Removal of Nitrate from Drinking Water by Carl-Ola Danielsson Department of Mechanics May 2006 Technical Reports from Royal Institute of Technology Department of Mechanics Fax´enLaboratoriet S-100 44 Stockholm, Sweden Typsatt i AMS-LATEX. Akademisk avhandling som med tillst˚and av Kungliga Tekniska H¨ogskolan i Stockholm framl¨agges till offentlig granskning f¨or avl¨aggande av teknologie dok- torsexamen torsdagen den 8:de juni 2006 kl 10.00 i sal D3, Kungliga Tekniska H¨ogskolan, Lindstedsv¨agen 5, Stockholm. c Carl-Ola Danielsson 2006 Tryck: Universitetsservice US AB, Stockholm 2006 Till¨agnad Far och Mor Electropermutation Assisted by Ion-Exchange Textile Removal of Nitrate from Drinking Water Carl-Ola Danielsson Fax´enLaboratoriet, Department of Mechanics, Royal Institute of Technology SE-100 44 Stockholm, Sweden. Abstract Increased levels of nitrate in ground water have made many wells unsuitable as sources for drinking water. In this thesis an ion-exchange assisted electromem- brane process, suitable for nitrate removal, is investigated both theoretically and experimentally. An ion-exchange textile material is introduced as a con- ducting spacer in the feed compartment of an electropermutation cell. The sheet shaped structure of the textile makes it easy to incorporate into the cell. High permeability and fast ion-exchange kinetics, compared to ion-exchange resins, are other attractive features of the ion-exchange textile. A steady-state model based on the conservation of the ionic species is devel- oped. The governing equations on the microscopic level are volume averaged to give macro-homogeneous equations. The model equations are analyzed and rel- evant simplifications are motivated and introduced. Dimensionless parameters governing the continuous electropermutation process are identified and their influence on the process are discussed. The mathematical model can be used as a tool when optimising the process parameters and designing equipment. An experimental study that aimed to show the positive influence of using the ion-exchange textile in the feed compartment of an continuous electroper- mutation process is presented. The incorporation of the ion-exchange textile significantly improves the nitrate removal rate at the same time as the power consumption is decreased. A superficial solution of sodium nitrate with a ini- tial nitrate concentration of 105 ppm was treated. A product stream with less than 20 ppm nitrate could be obtained, in a single pass mode of operation. Its concluded from these experiments that continuous electropermutation us- ing ion-exchange textile provides an interesting alternative for nitrate removal, in drinking water production. The predictions of the mathematical model are compared with experimental results and a good agreement is obtained. Enhanced water dissociation is known to take place at the surface of ion- exchange membranes in electromembrane processes operated above the limit- ing current density. A model for this enhanced water dissociation in presented in the thesis. The model makes it possible to incorporate the effect of wa- ter dissociation as a heterogeneous surface reaction. Results from simulations of electropermutation with and without ion-exchange textile incorporated are presented. The influence of the water dissociation is investigated with the developed model. vi Descriptors: Ion-exchange textile, Ion-exchange membrane, Electropermu- tation, Electroextraction, Electrodialysis, Electrodeionisation, Modeling, Con- ducting spacer, Nitrate removal, Water treatment, Water dissociation. Preface This thesis treats ion-exchange assisted electropermutation both theoretically and experimentally. The research was conducted within the framework of Fax´enLaboratoriet, a center of excellence in industrial fluid mechanics located at the Royal Institute of Technology in Stockholm, Sweden. Vattenfall AB has been the main industrial partner and parts of the work has been performed at Vattenfall Utveckling AB’s electrochemistry laboratory. The thesis is divided into two parts. In the first of these, an introduction to the process and a sum- mary of the research conducted is given in order to clarify its context. The second part consists of 4 appended scientific papers. Stockholm, May 2006 Carl-Ola Danielsson Appended articles: Paper 1. Carl-Ola Danielsson, Anders Dahlkild, Anna Velin & M˚arten Behm Nitrate Removal by Continuous Electropermutation Using Ion- Exchange Textile Part I: Modeling Published in Journal of The Electrochemical Society 153(4) D51-D61, 2006 Paper 2. Carl-Ola Danielsson, Anna Velin, M˚arten Behm & An- ders Dahlkild Nitrate Removal by Continuous Electropermutation Using Ion-Exchange Textile Part II: Experiments Published in Journal of The Elec- trochemical Society 153(4) D62-D67, 2006 Paper 3. Carl-Ola Danielsson, Anders Dahlkild M˚arten Behm & Anna Velin A Model for the Enhanced Water Dissociation On Monopolar Membranes. To be Submitted Paper 4. Carl-Ola Danielsson, Anders Dahlkild, Anna Velin & M˚arten Behm Modeling Continuous Electropermutation with Effects of Wa- ter Dissociation Included To be Submitted viii PREFACE Division of work between authors The work presented in this thesis has been done in collaboration with other researchers. The respondent has performed the major part of the work. Docent Anders Dahlkild, Department of Mechanics KTH, Dr. Anna Velin, Vattenfall Utveckling AB and Dr. M˚arten Behm, Department of Chemical Engineering and Technology, Applied Electrochemistry KTH, have acted as supervisors. They have all contributed with comments and discussions of the the work and the manuscripts. Parts of the modeling activities have been presented in a poster at, The 53rd Annual Meeting of the International Society of Electrochemistry, D¨usseldorf, Germany, in September 2002, and in a talk given at, The 205th meeting of the electrochemical society in San Antonio, Texas, U.S., in May 2004. Contents Preface vii Chapter 1. Introduction 1 Removal of Nitrate from drinking water 1 Background 3 Outline of thesis 4 Chapter 2. Ion-Exchange and Electromembrane Processes 5 Ion-exchange (IX) 5 Ion-exchange membrane processes 6 Electrodialysis (ED) 6 Electropermutation (EP) 8 Ion-Exchange assisted electromembrane processes 9 Ion-exchange textiles 13 Chapter 3. Modelling 14 Volume averaging 15 Conservation of mass 16 3.1. Enhanced Water Dissociation 20 Chapter 4. Experimental Investigations 22 Nitrate removal 22 Characterization of textile 24 Permeability 24 Conductivity of fiber bed 25 Chapter 5. Summary of Papers 30 Paper I 30 Paper II 33 Paper III 35 Paper IV 37 ix x CONTENTS Chapter 6. Concluding Discussion and Outlook 42 Concluding Discussion 42 Acknowledgment 45 Bibliography 46 Nitrate Removal by Continuous Electropermutation Using Ion- Exchange Textile Part I: Modeling Nitrate Removal by Continuous Electropermutationusing Ion- Exchange Textile as Conducting Spacer Part II: Experiments A Model for the Enhanced Water Dissociation On Monopolar Membranes Modeling Continuous Electropermutation with Effects of Water Dissociation Included CHAPTER 1 Introduction To obtain freshwater of high quality directly from the kitchen tap is something that many of us take for granted. We use it every day to prepare our food, to wash our clothes and for many other things. In Sweden the consumption of water is about 200 l of water per person per day [1]. Increasing environmental pollution has made many wells unsuitable as freshwater sources. Use of water treatment techniques is needed in order to meet society’s need of high quality water. The regulations on the water quality is continuously getting more and more strict as new and better analytical instruments are developed making it possible to detect lower and lower levels of impurities. What is regarded as good water quality depends on the application. Potable water should be free from toxic and harmful substances. Ultrapure water on the other hand, is not considered as high quality drinking water, where some minerals are desirable. The taste, smell and visual appearance of the water are other important aspects of drinking water quality. Furthermore, there are some technical aspects of a suitable drinking water that are considered. For example there are regulations on the pH and conductivity of the water in order to reduce corrosion problems in the pipes. The definition of clean water in many industrial applications is completely different compared to the potable water. The microelectronic and pharmaceu- tical industries require extremely pure water in their processes. In powerplants ultrapure water is used to reduce problems with corrosion that could be a se- rious problem at the temperatures and pressures present in the boilers. The production of this ultrapure water requires sophisticated water treatment sys- tems. For many industrial processes a zero waste target is on the agenda. Water treatment systems are used to reduce discharge of e.g. heavy metals for envi- ronmental reasons. There might also be an economical advantage if chemicals used in the process can be recycled. Removal of Nitrate from drinking water − The primary health concern regarding nitrate, NO3 ,isthatitisreducedto − nitrite, NO2 , in the body. Nitrite in turn reacts with the red blood cells to form methemoglobin, which affects the blood’s capability to transport oxygen. Infants are especially sensitive due to their low gastric acidity, which is favorable 1 2 1. INTRODUCTION for the reduction of nitrate. High intake
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