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Remediation of Acid Mine Drainage Using Natural Zeolite

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Remediation of Acid Mine Drainage Using Natural Zeolite REMEDIATION OF ACID MINE DRAINAGE USING NATURAL ZEOLITE By TAFADZWA MOTSI A thesis submitted to The University of Birmingham for the degree of DOCTOR OF PHILOSOPHY School of Chemical Engineering The University of Birmingham United Kingdom March 2010 University of Birmingham Research Archive e-theses repository This unpublished thesis/dissertation is copyright of the author and/or third parties. The intellectual property rights of the author or third parties in respect of this work are as defined by The Copyright Designs and Patents Act 1988 or as modified by any successor legislation. Any use made of information contained in this thesis/dissertation must be in accordance with that legislation and must be properly acknowledged. Further distribution or reproduction in any format is prohibited without the permission of the copyright holder. Abstract This research focuses on the removal of Fe, Cu, Zn and Mn from synthetic metal solutions and real AMD from Wheal Jane mine using natural zeolite. Laboratory experiments were performed to investigate the effectiveness of natural zeolite as a potential low cost material for the removal of these heavy metals from AMD. These include, equilibrium tests, batch kinetic studies, column studies and desorption studies. Equilibrium studies showed that the capacity of natural zeolite for heavy metals increased with an increase in initial solution pH. Fitting of the Langmuir and Freundlich isotherms to experimental data gave good fits, R2 values ranging from 0.9 – 0.99. The selectivity series of natural zeolite was: Fe3+>Zn2+>Cu2+>Mn2+. The amount of exchangeable cations increased at equilibrium, indicating that ion exchange had taken place. Higher metal uptakes were achieved by increasing agitation speed, initial solution pH, particle size reduction, and thermal pre-treatment. The rate limiting step for this process was intraparticle diffusion. Column studies showed that natural zeolite was capable of removing heavy metals from a continuously flowing solution. The breakthrough time increased with a longer bed height and slower flow rate. The bed depth service time model (BDST) was used to simulate experimental data and deviated from these by 12 – 14%. The treatment of actual Wheal Jane mine AMD showed that about 71-99% Fe and 97- 99% Cu were removed from solution. Results from the treatment of actual AMD revealed that natural zeolite was best suited for treating dilute metal solutions, and hence should be used downstream of other AMD treatment technologies. ii Dedication To my dearly beloved parents, Mr A. Motsi and Mrs L. Motsi, for their constant love, support and wisdom. iii Acknowledgements I would like to gratefully acknowledge the valuable assistance and encouragement I received throughout this project from my supervisors, Dr Neil Rowson and Dr Mark Simmons. I would also like to express my appreciation to IMERYS Minerals Ltd, UK for supplying the natural zeolite samples used in this project and their technical assistance in analysing some of these samples. I would also like to acknowledge the financial support I received from the Overseas Research Scholarship Award (ORSAS), which gave me the opportunity to carry out this project. I am grateful to my family for their support, love and encouragement. To my father for continually challenging me and reminding me to give it my best all the time. Special thanks to my mum for her refreshing words and love. To my young sister, Tatenda, thank you for being a continual inspiration. I am immensely grateful to my friends for their love, support and company without which this project would have been very difficult. Finally, I would like to give my heartfelt thanks to God for blessing me with the wonderful people that surrounded me during my study and also for blessing me with favour, strength and good health to complete it. iv Table of Contents Abstract……………………………………………………………………………………ii Dedication………………………………………………………………………………...iii Acknowledgement………………………………………………………………………..iv List of Figures…………………………………………………………………………….ix List of Tables……………………………………………………………………………xiii Nomenclature…………………………………………………………………………....xvi Chapter 1: Introduction 1.1 Evaluation of the Acid Mine Drainage Problem…………………………….………1 1.2 Treatment of Acid Mine Drainage…………………………………………………..3 1.3 Motivation and Aims of Thesis……………………………………………………...5 1.4 Thesis Structure…………………………………………………………...………...6 Chapter 2: Literature Review 2.1 Introduction………………………………………………………………………….9 2.2 Acid Mine Drainage……………………………………………………..…………10 2.2.1 Sources of Acid Mine Drainage……………………………………..………....10 2.2.2 Formation and Constituents of Acid Mine Drainage…………………..………11 2.2.3 Environmental and Ecological Impact of Acid Mine Drainage……………..…13 2.2.4 Preventing Acid Mine Drainage Formation………………………………..…..18 2.2.5 Technologies used for treating Acid Mine Drainage………………………..…20 2.2.6 Recovery of valuable products from AMD treatment………………………....30 2.3 Adsorption of Acid Mine Drainage…………………………………………..……31 2.3.1 Adsorption Process………………………………………………………..…...31 2.3.2 Examples of Adsorbents…………………………………………………..…...33 2.3.3 Natural Zeolite……………………………………………………………..…..34 2.3.3.1 Occurrence of Natural Zeolites……………………………………..……35 2.3.3.2 Framework and Structure of zeolites………………………………..…...37 2.3.3.3 Application of Natural Zeolites……………………………………..…...39 2.3.3.4 Using Natural Zeolite to treat Acid Mine Drainage………………..…….41 v Chapter 3: Case Study, Wheal Jane Mine 3.1 Brief History………………………………………………………………..……...43 3.2 Composition of Wheal Jane Mine AMD……………………………………..……45 3.3 Treatment technologies used at Wheal Jane Mine…………………………...…….46 3.3.1 Active Treatment………………………………………………………...…….46 3.3.2 Passive Treatment………………………………………………………...……47 3.4 Conclusion………………………………………………………………….…..….48 Chapter 4: Materials and Methods 4.1 Introduction…………………………………………………………………...……49 4.2 Materials and Sample Preparation……………………………………….……..….49 4.2.1 Synthetic solutions and other chemicals……………………………….…..…..49 4.2.2 Characterisation of Natural Zeolite……………………………………...……..50 4.3 Experimental Procedure………………………………………………………..…..53 4.3.1 Batch Adsorption Studies………………………………………………..…….53 4.3.2 Column Studies…………………………………………………………..…….57 4.3.3 Treatment of AMD from Wheal Jane Mine………………………………..…..59 4.4 Sample Analysis………………………………………………………………..…..60 Chapter 5: Characterisation of Natural Zeolite 5.1 Introduction…………………………………………………………………..…….62 5.2 Scanning Electron Microscopy (SEM)………………………………………….....63 5.3 Energy Dispersive Spectroscopy (EDS)……………………………………..…….69 5.4 X – Ray Diffraction …………………………………………………………..…...71 5.5 X – Ray Fluorescence..……………………………………………………..……...72 5.6 Other particle characteristics…………………………………………………..…...74 Chapter 6: Equilibrium Studies 6.1 Introduction…………………………………………………………………...……76 6.2 Equilibrium isotherms……………………………………………………………...77 6.2.1 Langmuir adsorption isotherm…………………………………………...…….77 6.2.2 Freundlich adsorption isotherm………………………………………..………79 vi 6.3 Results and discussion………………………………………………………..……80 6.3.1 Removal of copper………………………………………………………..…...80 6.3.2 Removal of zinc…………………………………………………………..……87 6.3.3 Removal of iron…………………………………………………………..……92 6.3.4 Removal of manganese……………………………………………………..….96 6.4 Selectivity of natural zeolite……………………………………………………...101 6.5 Conclusion………………………………………………………………………..104 Chapter 7: Kinetic Studies 7.1 Introduction………………………………………………………………………106 7.2 General Kinetic study results………………………………………………….….107 7.3 Factors that affect rate of Adsorption……………………………………….……109 7.3.1 Effect of adsorbent mass………………………………………….…….…….109 7.3.2 Effect of particle size………………………………………………….……...111 7.3.3 Effect of initial solution pH…………………………………………….…….113 7.3.4 Effect of initial solution concentration……………………………….………117 7.3.5 Effect of agitation…………………………………………………….………120 7.3.6 Effect of competing cations………………………………………….……….122 7.3.7 Effect of thermal pre – treatment……………………………………….…….124 7.4 Desorption/Regeneration studies………………………………………….……...128 7.5 Treatment of Synthetic Acid Mine Drainage (sAMD)………………….………..132 7.6 Kinetic Modelling………………………………………………………….……..135 7.6.1 Chemical Reaction control…………………………………………………...135 7.6.2 Film transfer diffusion control (external mass transfer)……………………...141 7.6.3 Intra – Particle diffusion control……………………………………………...146 7.6.4 Interruption Tests……………………………………………………………..153 7.7 Conclusion………………………………………………………………………..156 Chapter 8: Column Studies 8.1 Introduction……………………………………………………………….………158 8.2 Breakthrough Curves………………………………………………………….….160 8.3 Modelling of fixed bed columns…………………………………………….……163 vii 8.3.1 Bed depth service time model……………………………………….………..163 8.3.2 Results and discussion………………………………………………………..165 8.4 Column operation…………………………………………………………………168 8.4.1 Effect of flow rate…………………………………………………………….168 8.4.2 Effect of bed height…………………………………………………………...171 8.5 Treatment of synthetic acid mine drainage (sAMD)……………………………..175 8.5.1 Adsorption studies……………………………………………………………175 8.5.2 Desorption studies…………………………………………………………….179 8.6 Conclusion………………………………………………………………………..183 Chapter 9: Treatment of Wheal Jane AMD 9.1 Introduction……………………………………………………………………….185 9.2 Batch Experiments………………………………………………………………..186 9.2.1 Use of thermally pre – treated natural zeolite in treating real AMD…………186 9.2.2 Standing tests for the treatment of Wheal Jane AMD………………………..189 9.2.3 Comparison between natural zeolite and synthetic zeolite in treating Wheal Jane mine AMD……………………………………………………………………194 9.2.4 Proposed design of a passive AMD
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