METAL RECOVERY FROM ELECTRONIC WASTE: TWO-STEP BIOLOGICAL AND CHEMICAL LEACHING FOR THE RECOVERY OF COPPER AND GOLD FROM ELECTRONIC WASTE Arda Işıldar Joint PhD degree in Environmental Technology Docteur de l’Université Paris-Est Spécialité : Science et Tech nique de l’Environnement Dottore di Ricerca in Tecnologie Ambientali Degree of Doctor in Environmental Technology Tesi di Dottorato – Thèse – PhD thesis Arda Işıldar Two-step biological and chemical leaching for the recovery of copper and gold from electronic waste th Defended on November 18 , 2016 In front of the PhD committee Professor Erkan Şahinkaya Reviewer Associate Professor Jaco Huisman Reviewer Associate Professor Ester van der Voet Reviewer Doctor Fritz Holzwarth Examiner Professor Piet N. L. Lens Promotor Associate Professor Eric D. van Hullebusch Co-Promotor Associate Professor Giovanni Esposito Co-Promotor 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: Dr. Hab. Eric D. van Hullebusch Hab. Associate Professor of Biogeochemistry Université Paris-Est Marne-la-Vallée, Paris, France Dr. Giovanni Esposito Associate Professor of Sanitary and Environmental Engineering Università degli Studi di Cassino e del Lazio Meridionale, Cassino, Italy Other members: Prof. Erkan Şahinkaya Professor of Environmental Engineering Faculty of Bioengineering, Istanbul Medeniyet Üniversitesi, Istanbul, Turkey Dr. Jaco Huisman Associate Professor of Design for Sustainability and Product Innovation Management Faculty of Industrial Design Engineering, TU Delft, Delft, the Netherlands Dr. Ester van der Voet Associate Professor of Industrial Ecology Institute of Environmental Sciences (CML), Leiden University, Leiden, the Netherlands Dr. Fritz Holzwarth Rector ad interim of UNESCO-IHE UNESCO-IHE Institute for Water Education, Delft, the Netherlands This research was conducted under the auspices of Erasmus Mundus Joint Doctorate Environmental Technologies for Contaminated Solids, Solids and Sediments (ETeCoS3) and the Graduate School for Socio-Economic and Natural Sciences of the Environment (SENSE) CRC Press/Balkema is an imprint of the Taylor & Francis Group, an informa business © 2018, Arda IŞILDAR Although all care is taken to ensure integrity and the quality of this publication and the information herein, no responsibility is assumed by the publishers, the author nor IHE Delft for any damage to the property or persons as a result of operation or use of this publication and/or the information contained herein. A pdf version of this work will be made available as Open Access via http://repository.tudelft.nl/ihe This version is licensed under the Creative Commons Attribution-Non Commercial 4.0 International License, http://creativecommons.org/licenses/by-nc/4.0/ Published by: CRC Press/Balkema Schipholweg 107C, 2316 XC, Leiden, the Netherlands [email protected] www.crcpress.com – www.taylorandfrancis.com ISBN 978-0-367-08705-0 ’’Look deeper into the nature, and then you will understand everything better.’’ Albert Einstein Acknowledgments This PhD work would have not been successfully and joyfully completed without the contributions of many exceptional people, who made this research a life experience rather than a mere research project. My sincere gratitude goes to my promoter Prof. Piet N.L. Lens who acutely dedicated his time, effort and valuable experience to this particular research project. My academic path and learning journey would not have shaped without his indispensable mentorship, training and guidance. When it comes to gratitude, my co-promoter Prof. Eric D. van Hullebusch deserves a special reservation, who undeniably formed my professional development and helped me open many new frontiers in my career. Without doubts, Eric will remain a lifelong counsel, an esteemed colleague, and a friend, beyond this PhD project. The contribution of Dr. Eldon Rene shaped the skeleton of this PhD work and bequeathed virtually all parts of this journey. His outstanding ability to balance professionalism and extracurricular activities made an excellent example of an esteemed researcher and chemical engineer. Dr. Jack van de Vossenberg was a source of inspiration, without whom this work would have not been completed, and a keen, detail-oriented, critical reviewer of scientific findings. Dr. Venkata Nancharaiah Yarlagadda facilitated the laboratory sessions in the best way any PhD fellow can dream of. Prof. Giovanni Esposito was always promptly available for any issue that may rise, and organized the enjoyable Summer School evenings in Cassino. Thank you, Giovanni, for coordinating the ETeCoS3 programme. The data would have not been accurately delivered without the tireless support of Ferdi, Peter Frank, Berend, Fred in Delft, and Chloé and Yoan in Paris. Especially the impressive teamwork of the UNESCO-IHE lab staff showed that a whole was more than the sum of its individual parts. I had the exceptional privilege to work with excellent M.Sc. students Bienvenu Mizero, Thresa Musongo, Marco Villares, Yaowen Wang, and Nuria Caseres. Neither the data would have been comprehensive, nor the discussion would have been in-depth without their valuable contribution. Special thanks go to Mr. Marco Villares, who not only shaped the course of this Acknowledgements | xii PhD work but also became an indispensable companion in professional and off-work environments. Many thanks to all the ETeCoS3 and ABWET colleagues; Chiara, Joy, Rohan, Suthee, Carlos, Susma, Anna, Manivannan, Lucian, Joana, Clement, Soliu, Douglas, Francesco, Ludovico, Kirki, Lea, Shrutika, Suchanya, Anna, who are not only fellow researchers but also friends and a source of a collective aura. The Summer Schools would have not been the same without the spontaneous sangria parties. Friends scattered around cities; Eirini, Iosif, Marco, Chris, Paulo, Mohaned, Alex, Poolad, Paolo, Maria, Sanaz, Ali, Germana, Angélica, Paulo, Maria, Nico, Veronica, Xiaoxia, Alessandra, Ekin, Omar, I celebrate our lifelong friendship built on invaluable memories acquired in Delft, Leiden, Paris and Cassino. Special thanks go to the colleagues at SIMS Recycling in Eindhoven, and at UNESCO-IHE IT department, colleagues at UNESCO-IHE, and the citizens of city of Delft for kindly providing the WEEE samples. And finally, I would like to address my appreciation to the sponsor of this work, the European Commission, which financially supported the project. Summary The well-being of the society depends on a number of metals, including base metals, precious metals and increasingly rare earth elements (REE). The usage of these metals increased in numerous applications, including electrical and electronic equipment (EEE), and their interrupted supply is at stake. There is an increasing interest in the secondary sources of these metals, particularly waste electrical and electronic equipment (WEEE) in order to compensate their potential supply deficit. This PhD thesis demonstrates the advantages and bottlenecks of biological and chemical approaches, as well as the advances and perspectives in the development of sustainable processes for metal recovery from WEEE. Furthermore, a novel process for the recovery of metals from WEEE is described, and a techno-economic assessment is given. Discarded printed circuit boards (PCB) from personal computers (PC), laptops, mobile phones and telecom servers were studied. Following an extensive literature review, a novel characterization and total metal assay method was introduced and applied to waste board materials. Discarded PCB contained metals in the range of (%, by weight): copper (Cu) 17.6 - 39.0, iron (Fe) 0.7 - 7.5, aluminum (Al) 1.0 - 5.5, nickel (Ni) 0.2 - 1.1, zinc (Zn) 0.3 - 1.2, as well as gold (Au) (in ppm) 21 - 320. In addition, multi-criteria analysis (MCA) using the analytical hierarchical process (AHP) methodology was applied for selection of the best-suited technology. A proof-of-concept for a two-step bioleaching extraction is given, in which 98.4% and 44.0% of the Cu and Au, respectively, were extracted. The two-step extraction procedure was applied to the chemical leaching of metals from PCB. Cu leaching was carried in an acidic oxidative mixture of H2SO4 and H2O2, whereas Au was leached by in a medium, 2− + catalyzed by CuSO4. Under the optimized conditions, 99.2% andS 29O23.2% ofN CHu4 and Au, respectively, were extracted from the board material. Selective recovery of Cu from the bioleaching leachate using sulfidic precipitation and electrowinning is studied. Cu was selectively recovered on the cathode electrode at a 50 mA current density in 50 minutes, with a 97.8% efficiency and 65.0% purity. The techno-economic analysis and environmental sustainability assessment of the new technology at an early stage of development was investigated.