METAL REMOVAL AND RECOVERY FROM MINING WASTEWATER AND E-WASTE LEACHATE Cu Ni Zn SUTHEE JANYASUTHIWONG Metal Removal and Recovery from Mining Wastewater and E-Waste Leachate Thesis Committee Thesis Promotor Prof. dr. ir. Piet N.L. Lens Professor of Biotechnology UNESCO-IHE Institute for Water Education Delft, The Netherlands Thesis Co-Promotors Prof. Michel Madon University of Paris-Est Paris, france Dr. Giovanni Esposito, PhD, MSc Assistant Professor of Sanitary and Environmental Engineering University of Cassino and Southern Lazio Cassino, Italy Dr. Hab. Eric D. van Hullebusch, PhD, MSc Hab. Associate Professor in Biogeochemistry University of Paris-Est Paris, france Mentor Dr. Eldon R. Rene UNESCO-IHE Institute for Water Education Delft, The Netherlands Reviewers Prof. Marie-Odile Simonnot University of Lorraine Nancy, France Prof. Ajit P. Annachhatre Asian Institute of Technology Pathumthani, Thailand This research was conducted under the auspices of the Erasmus Mundus Joint Doctorate Environmental Technologies for Contaminated Solids, Soils and Sediments (ETeCoS3) and The Netherlands Research School for the Socio-Economic and natural Sciences of the Environment (SENSE). JJooiinntt PPhhDD ddeeggrreeee iinn EEnnvviirroonnmmeennttaall TTeecchhnnoollooggyy Doctuer de l'Université Paris-Est SSppéécciiaalliittéé :: SScciieennccee TTeecchhnniiqquuee ddee ll''EEnnvviirroonnnneemmeenntt DDoottttoorree ddii RRiicceerrccaa iinn TTeeccnnoollooggiiee AAmmbbiieennttaallii DDeeggrreeee ooff DDooccttoorr iinn EEnnvviirroonnmmeennttaall TTeecchhnnoollooggyy TThhèèssee - Tesi di Dottorato - PhD Thesis Suthee Janyasuthiwong MMeettaall RReemmoovvaall aanndd RReeccoovveerryy from Mining Wastewater aanndd EE-Waste Leachate defended 3 July 2015 In front of the PhD committee PPrrooff.. ddrr.. iirr.. PPiieett NN.. L. Lens Promotor PPrrooff.. MMiicchheell MMaaddoonn Co-Promotor DDrr.. GGiioovvaannnnii EEssppoossiittoo Co-Promotor DDrr.. HHaabb.. EErriicc DD.. vvaann HHuulllleebbuusscchh Co-Promotor DDrr.. EEllddoonn RR.. RReennee Mentor Prof. Ajit P. AAnnnnaacchhhhaattrree Reviewer Prof. Marie-OOddiillee Simonnot Reviewer EEErrraaasssmmmuuusss MMMuuunnnddduuusss JJJoooiiinnnttt DDDoooccctttooorrraaattteee ppprrrooogggrrraaammm iiinnn EEEnnnvvviiirrrooonnnmmmeeennntttaaalll TTTeeeccchhhnnnooolllooogggiiieeesss fffooorrr CCCooonnntttaaammmiiinnnaaattteeeddd SSSooollliiidddsss,,, SSSoooiiilllsss aaannnddd Sediments (ETeCoS ) 3 CRC Press/Balkema is an imprint of the Taylor & Francis Group, an informa business © 2015, Suthee Janyasuthiwong All rights reserved. No part of this publication or the information contained herein may be reproduced, stored in a retrieval system, or transmitted in any form or by any means, electronic, mechanical, by photocopying, recording or otherwise, without written prior permission from the publishers. Although all care is taken to ensure the integrity and quality of this publication and information herein, no responsibility is assumed by the publishers or the author for any damage to property or persons as a result of the operation or use of this publication and or the information contained herein. Published by: CRC Press/Balkema PO Box 11320, 2301 EH Leiden, The Netherlands e-mail: [email protected] www.crcpress.com – www.taylorandfrancis.com ISBN 978-1-138-02949-1 (Taylor & Francis Group) Table of Contents Chapter Title Page Acknowledgements vi Summary vii Samenvatting ix Sommario xi Résumé xiii 1 General Introduction 1 2 Metal Rich Waste Stream and Feasibility of Recovery 8 3 Adsorption Technology for Metal Contaminated Wastewater 33 Treatment 4 The Performance of Sulfate Reducing Bacteria Biotechnology in 59 an Inverse Fluidized Bed Bioreactor 5 Inversed Fluidized Bed SRB Bioreactor for Metal Contaminated 86 Wastewater Treatment 6 Effects of Process Parameter on Metal Yield in E-waste Leachate 104 7 General Discussion 124 The Netherlands Research School for the Socio-Economic and 141 Natural Sciences of the Environment (SENSE) certificate Curriculum Vitae 143 Publications and Presentations 144 v Acknowledgements First of all, I would like to express my sincere gratitude toward my promotor, Prof. Piet N. L. Lens, for his kindness to give me an opportunity to do this research under his supervision. Moreover, I would like to extend my gratitude to Dr. Giovanni Esposito and Dr. Hab. Eric D. van Hullebusch, my co-promotors, for their help during my ETeCoS3 program. I would like to give my greatest appreciation towards my mentor, Dr. Eldon R. Rene, who was always there to help me throughout my PhD phase. With his help, encouragement and support, both in academic and non-academic paths, my thesis has become a big success. I would like to also extend my gratitude towards two of my external thesis reviewers Prof. Ajit P. Annachhatre and Prof. Marie-Odile Simonnot for showing interest in my works. With their kind suggestions and valuable feedbacks, aimed at addressing the practical implications, the thesis contents were largely improvised. Moreover, I would like to thank Prof. Vera Susanne Rotter for her kind help in processing the e-waste materials and her constructive suggestions for my research. I would like to thank two of the master students, Sheila Monica Phiri (deceased) and Riccardo Ugas, for their contribution towards this research. Their hard work and perseverance paved the way to publish good quality manuscripts. In addition, they also helped me to understand the practical difficulties of this research, its limitations and above all taught me - how to be a good mentor. Sheila, you are my first master student; thanks for your big heartedness and we will always remember you for that in our prayers. I also had the opportunity to spend the time when you won the MSc research competition at IHE. Thanks to you too, Riccardo, even though we had limitations to finish your project, you still kept working to the best of your abilities and successfully completed your MSc thesis. Moreover, I would like to thanks all my colleagues for their friendship and support during tough times. I would like to thank Fred Kruis, Frank Wiegman, Ferdi Battes, Lyzette Robbemont, Peter Heerings, Berend Lolkema and Don van Galen for their help and support in the laboratory. Thanks to Rohan Jain, Purvi Jain, Erika Espinosa Ortiz and Estefanía López for their wonderful friendship which made my PhD life enjoyable. I really appreciate the time we all went out together, whether it was for a summer school or a short course or to relax. I still feel like, it was just yesterday when we were together even though we walk in different paths now. I also would like to thank Silvio Matassa and Marta Cardile who made my journey (mobility) to Italy commending. Thank to the fellowship from Erasmus Mundus Joint Doctorate program in Environmental Technology for Contaminated Solids, Soils and Sediments (ETeCoS3) which give me this big opportunity to finish my PhD. With their supports, my overall world view has widened and I can see how people endure in this small world and I got to know people's attitudes better (positive and negative). Thus, this PhD stint served as a valuable experience in my life/career. Lastly, I whole heartedly thank my dear family living in Thailand who constantly provided me the kind support, motivation and encouragement, during the good and bad times I had to face. Thanks to my mother and brother who let me to prosper in my educational career and cherish my own dream which they had to endure from a distance. Suthee Janyasuthiwong (September, 2015) vi Summary (English) Metal contamination in the environment is one of the persisting global issues since it not only disturbs the environmental quality, but also the environment and human health. The major contribution to this problem arises mainly from anthropogenic activities such as industries. Metal scarcity has become more severe lately where some elements have been predicted to be eradicated from the earth crust in several decades. Recently, researchers have focused their attention to recover these metals from the waste stream and reuse it in industrial production processes. The use of agricultural wastes as a potential low cost adsorbent for heavy metal removal from wastewater is one of the most versatile technologies. In this study among the different adsorbents tested, groundnut shell gave high removal efficiencies with fewer requirements for further post treatment for Cu, Pb and Zn removal. Furthermore, the batch experiments on the main effects of process parameters (pH, adsorbent dosage, contact time and initial metal concentration) showed a major effect on the metal uptake and removal efficiency. For material regeneration, 0.2 M HCl was the most effective desorbing solution that did not alter the efficiency, up to three adsorption and desorption cycles. The use of sulfate reducing bacteria (SRB) in bioreactors is another technology that can be applied for the treatment of metal contaminated wastewater. The SRB reduce sulfate into sulfide which further reacts with metals to form metal sulfide precipitates. The inverse fluidized bed (IFB) bioreactor is a configuration which shows prominence in utilizing SRB technology for metal contaminated wastewater treatment. Two IFB bioreactors were operated at different pH (7.0 and 5.0). The sulfate reducing activity (SRA) at pH 7.0 was higher than at pH 5.0, illustrating that pH is the main factor that affects SRA. However, thiosulfate showed a higher efficiency than sulfate as an alternate electron acceptor. The sulfide produced using thiosulfate as the electron acceptor was 157.0 mg/L, while only 150.2 mg/L was produced using sulfate and it required an adaptation period at pH 5.0 prior to successful operation. Moreover, the IFB showed a high efficiency for Cu, Ni and Zn removal from synthetic wastewater. The removal of Cu and Zn was more than 90% at pH 7.0 and 5.0 at an initial metal concentration of 25 mg/L. On the other hand, Ni was not removed at an initial concentration of 25 mg/L, as it exerted toxic effects towards SRB. There are various types of metal contaminated waste streams which pose as a good candidate for metal recovery include electronics waste (e-waste). This e-waste has a high potential as vii secondary source of metal to recover especially base metals such as Cu, Ni and Zn. Printed circuit boards (PCBs) of personal computers were evaluated as the potential secondary source of Cu, Ni and Zn using hydrometallurgical and sulfide precipitation methods. The optimal conditions for metal leaching were 0.1 M HNO with a liquid to solid ratio of 20 using PCBs 3 of 0.5 - 1.0 mm particle size at 60 °C, which resulted in 400 mg Cu/g PCBs. With sulfide precipitation at a stochiometric ratio of 1:1 (Cu:S2-), the recovery of Cu was very effective up to 90% from the leachate which accounted to approximately 0.41 g Cu/g PCBs, while Ni and Zn recovery were, respectively, 40% (0.005 g Ni/g PCBs) and 50% (0.006 g Zn/g PCBs) from the leachate in an upflow leaching column. viii