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Sustainable Nanotechnology: Life Cycle Thinking in Gold Nanoparticle Production and Recycling

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Sustainable Nanotechnology: Life Cycle Thinking in Gold Nanoparticle Production and Recycling Sustainable Nanotechnology: Life Cycle Thinking in Gold Nanoparticle Production and Recycling Paramjeet Pati Dissertation submitted to the faculty of the Virginia Polytechnic Institute and State University in partial fulfillment of the requirements for the degree of Doctor of Philosophy In Civil Engineering Peter J. Vikesland (Chair) Sean P. McGinnis (Co-chair) Linsey C. Marr Amy Pruden Scott H. Renneckar August 4, 2015 Blacksburg, Virginia Keywords: nanotechnology, LCA, recycling, gold, sustainability Sustainable Nanotechnology: Life Cycle Thinking in Gold Nanoparticle Production and Recycling Paramjeet Pati ABSTRACT Nanotechnology has enormous potential to transform a wide variety of sectors, e.g., energy, electronics, healthcare, and environmental sustainability. At the same time, there are concerns about the health and environmental impacts of nanotechnology and uncertainties about the fate and toxicity of nanomaterials. Life cycle assessment (LCA), a quantitative framework for evaluating the cumulative environmental impacts associated with all stages of a material or process, has emerged as a decision-support tool for analyzing the environmental burdens of nanotechnology. The objective of this research was to combine laboratory techniques with LCA modeling to reduce the life cycle impacts of gold nanoparticle (AuNP) production. The LCA studies were focused on three aspects of AuNP synthesis: 1) the use of bio-based (‘green’) reducing agents; 2) the potential for recycling gold from nanomaterial waste; and, 3) the reduction of the life cycle impacts of AuNP production by conducting the synthesis at reduced temperature. The LCA models developed for AuNPs can inform future nanotechnology-focused LCA studies. Comparative LCA showed that in some cases, the environmental impacts associated with green synthesis methods may be worse than those of conventional synthesis approaches. The main driver of the environmental burdens associated with AuNP synthesis is the large embodied energy of gold, and so-called green synthesis methods do not offset those impacts. In addition, the reaction yield, which is seldom reported in the literature for green synthesis of nanomaterials, was found to greatly influence the life cycle impacts of AuNP synthesis. Gold from nanomaterial waste was successfully recovered by using host-guest inclusion complex formation facilitated by - cyclodextrin. This recycling approach involved room temperature conditions and did not require the toxic cyanide or mercury commonly used in the selective recovery of gold. A major advantage offered by this approach for selective gold recovery over conventional approaches is that the recovery does not involve the use of toxic cyanide or mercury. To reduce the energy footprint of citrate-reduced AuNP synthesis, the synthesis was conducted at room temperature. LCA models showed significant reduction in the energy footprint. The findings of this research can inform future LCAs of other nanomaterials. DEDICATION “The greatest obstacle to discovering the shape of the earth, the continents, and the oceans was not ignorance but the illusion of knowledge.” -Daniel J. Boorstin “One accurate measurement is worth a thousand expert opinions.” -Grace Hopper “I am recycled cells I learn to like myself More with each iteration I’m an experiment Each trial is a test Constant recalibration” -Sarah Daly (Iterations) Metaphorest iii ACKNOWLEDGEMENTS My Ph.D. journey is dotted with the kindness, support and generosity of several mentors, colleagues and friends. I owe my deepest gratitude to Dr. Peter Vikesland, my primary advisor, for his guidance, support and encouragement throughout my graduate studies at Virginia Tech. Pete: Thanks for pushing me to strive for high-quality work and for constantly raising the bar. You trusted me when I had grave doubts about myself and my seemingly insane research plans, and you gave me ample room to experiment with ideas and to pursue my own intuitions and research interests. I owe much of my growth as an independent researcher to the fecund research environment, the generous resources and the numerous opportunities you provided. Dr. Sean McGinnis, my co-advisor, played a major role in helping me develop my life cycle thinking muscles and LCA modeling skills. Dr. McGinnis: Our many conversations about sustainability helped me refine my ideas about the many meanings and interpretations of the deceptively simple word sustainable. Those conversations also helped me develop a systems approach for thinking about the wicked complexities at the intersection of environmental sustainability, economics and ethics. I also appreciate your insights and advice about the nuts and bolts of teaching. I would also like to thank my committee members Dr. Linsey Marr, Dr. Amy Pruden and Dr. Scott Renneckar for their ideas and suggestions, which gave this dissertation its final shape. I will continue to incorporate your recommendations as I move my research projects forward. This research would not have been possible without the facilities and resources provided by the Department of Civil and Environmental Engineering (CEE), the Virginia Tech Center for Sustainable Nanotechnology (VTSuN), and the Nanoscale Characterization and Fabrication Laboratory (NCFL). I am especially grateful to Chris Winkler for his many hours of help at the NCFL. Chris: Thank you for your boatloads of patience, as I tried my inexperienced, shaky, and over-caffeinated hands at transmission electron microscopy. You made the NCFL inviting and TEM less frightening – even fun. On behalf of all the eager researchers who show up at the NCFL with samples, clueless about TEM but reassured that they have Chris to guide them - I thank you. I owe a huge thanks to Julie Petruska, for sharing with me her encyclopedic knowledge of lab protocols and safety practices, and for helping me find obscure chemicals, lab equipment, and glassware. Julie: Thanks to your help and suggestions in designing experiments that involved aqua regia, hydrobromic acid and other unsavory chemicals, I successfully managed to not poison, dissolve or vaporize myself even once. iv During my Ph.D., I got to work with and to mentor two amazing undergraduate researchers – Jennifer Kim and Leejoo Wi. Jennifer and Lee: By working with you, I have learnt so much about mentoring. Your hard work has helped me move multiple research projects forward. I wish you both the very best. I was fortunate to be a part of the Environmental Nanoscience and Technology (ENT) Lab. In my fellow ENTs, I found an incredibly supportive group of friends and colleagues with whom I shared so many conversations, rants, and laughs. Andrea: Thank you for all the thought-provoking conversations and brainstorming sessions about the role of ethics in engineering, the state of academia, the cultural lenses through which we view life... Thanks also for the aloo paranthas, rice and dal that kept me nourished and alive when I fell ill before the defense. Bahut bahut dhanyavaad. Virginia: Thanks to you too for the many conversations and for having me in your team during the softball matches. With my hand-eye coordination (or lack of thereof), I did not have much to contribute in terms skills. But I had a lot of fun even as I stayed perpetually confused about the rules. You bring a special joy, and you should know that everyone in the lab thinks we should clone you and paradrop your clones all over the globe – the world will be a happier place. Nina: Thanks for your initiative and commitment to VTSuN. You play multiple roles for VTSuN - the engine, the steering wheel, the navigation system, and sometimes all three simultaneously – and make it all seem annoyingly effortless. I am in awe at your efficiency, creativity, vision and execution, and am always inspired (and very jealous). VTSuN is lucky to have you. Weinan: You have taught me so much about lab work, designing experiments, and thinking through research problems. It was a pleasure working with you and learning from you, and is an honor to have you as my colleague and friend. Andrea, Nina, Ron, Matt (Chan), Matt (Hull), Becky, Hossein, Haoran, Marjorie, Virginia, and Weinan – it was a pleasure. My project with Sheldon Masters on the role of ethics in environmental engineering education was one of the highlights of my Ph.D. experience. Sheldon: I could not have done it without you. Thanks for the many meals, conversations and lightbulb-in-the-head-switching-on moments. I would also like to express my gratitude to Matthew Grice in the Graduate School for reviewing this dissertation draft for formatting issues during one of his busiest times in the year. v No amount of graduate training could have prepared me to handle my arch nemeses that have always worried, flummoxed and frustrated me – HokieMart and paperwork. I am deeply indebted to Beth Lucas (EWR) for helping me to navigate the maze of paperwork, solve fiendishly knotty HokieMart-related puzzles, and for alerting me to upcoming deadlines that would have blindsided and derailed me. I am also very grateful to Leigh Anne Byrd (formerly in CEE, currently in Pamplin College) for all her help with scheduling my preliminary and final exams, and for expediting the paperwork related to those. Beth and Leigh Anne: Thank you so much for always coming through. My acceptance into the CEE Ph.D. program at Virginia Tech was made possible by the education, mentorship and nurturing guidance I received from Dr. Masten at Michigan State University. Dr. Masten: The lessons I learnt from you at MSU have always stayed with me. Not only lessons in thinking, reasoning, writing, and scientific rigor, but also lessons in resilience, kindness and humility that I picked up from you when you not looking, but were busy being resilient, kind and humble. Forever grateful. A lot has changed in these last five years. Thankfully, as I made my way through the ebb and flow of temporary setbacks and lucky breaks, what remained unchanged was the reassuringly constant love and unwavering support of my family and friends in India.
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