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Fate and Reactivity of Natural and Manufactured Nanoparticles in Soil/Water Environments Allison Vandevoort Clemson University, [email protected]

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Clemson University TigerPrints All Dissertations Dissertations 12-2012 Fate and Reactivity of Natural and Manufactured Nanoparticles in Soil/Water Environments Allison Vandevoort Clemson University, [email protected] Follow this and additional works at: https://tigerprints.clemson.edu/all_dissertations Part of the Environmental Sciences Commons Recommended Citation Vandevoort, Allison, "Fate and Reactivity of Natural and Manufactured Nanoparticles in Soil/Water Environments" (2012). All Dissertations. 1018. https://tigerprints.clemson.edu/all_dissertations/1018 This Dissertation is brought to you for free and open access by the Dissertations at TigerPrints. It has been accepted for inclusion in All Dissertations by an authorized administrator of TigerPrints. For more information, please contact [email protected]. FATE AND REACTIVITY OF NATURAL AND MANUFACTURED NANOPARTICLES IN SOIL/WATER ENVIRONMENTS A Dissertation Presented to the Graduate School of Clemson University In Partial Fulfillment of the Requirements for the Degree Doctor of Philosophy Plant and Environmental Sciences by Allison René Rick VandeVoort December 2012 Accepted by: Dr. Yuji Arai, Committee Chair Dr. John Andrae Dr. Cindy Lee Dr. Horace Skipper ABSTRACT Nanoparticles (NPs), < 100 nm in diameter, make up the smallest component of solid material. This small size often causes increased reactivity in soil/water environments, which is true for both natural NPs, such as very fine clay particles, and for manufactured nanoparticles, such as silver nanoparticles (AgNPs). As the importance of these particles is more widely recognized, and as manufactured nanoparticles, especially AgNPs, are increasing in production, it is essential to consider their effect on terrestrial and aquatic environments. The studies presented in this dissertation show that both the physicochemical characteristics of the NPs (e.g., particle size, surface coating, elemental composition), as well as soil-water interfacial chemistry (e.g., ionic strength, ligand concentration, pH), are instrumental in predicting environmental fate and reactivity. Ligand type and concentration were especially important in NP reactivity and bioavailability. Using the hard/soft acid/base concept, the effect of phosphate ligand (hard base) on Fe/Al (hard acid) oxyhydroxide natural NPs was investigated in Chapters 2 and 3. Adding phosphate to soil NPs and reference nano-minerals (Fe-(oxyhydr)oxides and kaolinite) caused coagulation or dispersion, changing the particle size of the NPs, as well as affecting the amount of phosphate in its bioavailable (i.e., dissolved) form. A review of the literature in Chapters 1 and 3 revealed that changes in the soil conditions, and therefore, soil colloids/NPs (e.g., increasing organic matter via amendments), also has a direct impact on the soil NP-facilitated phosphate transport processes. ii Silver, a soft acid, reacts readily with thiol functional groups, soft bases, in humic substances prevalent in soil environments. The effect of soil constituents on AgNP reactivity and phase transformation was investigated in Chapters 4 and 5. The presence of solid surfaces facilitated sorption and phase transformation in all AgNPs studied over the course of 30 days, especially when compared to the same AgNPs aged in aqueous environments in the absence of soil. When the bioavailability of Ag (as ionic and NPs), a known antimicrobial agent, was assessed via denitrification experiments in Chapter 5, the AgNPs exhibited much less toxicity than expected, perhaps due to their strong sorption onto soil particles, as observed in the adsorption isotherm experiments conducted in Chapter 4. A more in-depth study of Ag(I) and AgNPs, and their interactions with cysteine, an amino acid with a thiol functional group, at the goethite-water interface in Chapter 6 revealed that, while cysteine enhanced the sorption of Ag(I) on goethite surfaces by forming inner-sphere ternary surface complexes, AgNP sorption to goethite was largely unaffected by cysteine. The behavior suggests hydrophobic interactions of AgNPs on goethite surfaces, revealing the effects of a soft ligand on Ag are via species specific (Ag(I) or AgNPs) mineral interactions, and are important in predicting AgNP fate in soil systems. This dissertation provides a novel viewpoint of natural and manufactured NP interactions in soil environments. These interactions are dictated by both particle-specific iii characteristics and environmental conditions. When environmental conditions, especially the presence of reactive ligands (based on the hard/soft acid/base theory), are altered by anthropogenic or indigenous means, the reactivity of certain NPs changes dramatically, impacting the bioavailability of contaminants such as phosphate, Ag(I), or AgNPs. iv DEDICATION To my parents, who, as my first teachers, instilled in me a love of learning and endless curiosity; and who have always given me unconditional love and support. And to Rob, for following me to South Carolina and giving me love and patience when I needed it most. v ACKNOWLEDGEMENTS The work presented in this dissertation would not have been possible without the help and guidance of many people. First and foremost, I would like to thank my advisor, Dr. Yuji Arai, for his continuous support and guidance through my doctoral studies. I also thank my committee members Dr. John Andrae, Dr. Cindy Lee, and Dr. Horace Skipper. The experiments carried out in this project were successful due, in large part, to the assistance of the following people: Dr. Brian Powell, for the use of zeta-potential, dynamic light scattering, and ICP-MS instruments, and for guidance taking measurements; Dr. Simon Scott, for assistance with and use of the ultra-high-speed centrifuge; Dr. Tanju Karanfil, and Onur Apul for BET surface area measurements; the entire staff of the Clemson Electron Microscope Facility, especially Dr. JoAn Hudson, Dr. Taghi Darroudi, and Dr. Haijun Qian; Aaron Edgington and Kim Newton for assistance with particle size measurements on equipment maintained by the Clemson University Environmental Toxicology Program; and Kathy Moore at Clemson Agricultural Services, for ICP-AES measurements. Special thanks also go out to the faculty and staff of the National Synchrotron Light Source at Brookhaven National Laboratory and the Stanford Synchrotron Radiation Lightsource, at which synchrotron- based measurements were conducted; in particular Dr. Antonio Lanzirotti and Dr. Ryan Tappero. In addition, I would like to thank my lab mates and other friends in the graduate school at Clemson University, for their encouragement and support. vi I wish to thank my family, especially my parents Douglas and Kyle Rick, for their unending support of my goals and education. I would not be the person I am today without their love, and the many opportunities they were able to provide for me. Finally, thank you to my husband, Robert VandeVoort, for his encouragement, assistance, patience, and love. This work was funded by the Clemson University Public Service in Agriculture Fellowship and the 2011 Agriculture and Food Research Initiative Competitive Grants Program, Nanotechnology for Agriculture and Food systems (#2011-03580). vii TABLE OF CONTENTS Page TITLE PAGE .................................................................................................................... i ABSTRACT ..................................................................................................................... ii DEDICATION ................................................................................................................. v ACKNOWLEDGEMENTS ............................................................................................ vi LIST OF TABLES .......................................................................................................... xi LIST OF FIGURES ....................................................................................................... xii CHAPTER 1. INTRODUCTION AND LITERATURE REVIEW ..................................... 1 1.1. Nanoparticles ............................................................................... 1 1.2. Phosphorus in Soil/Water Environments ..................................... 2 1.3. Silver in Soil/Water Environments ............................................ 33 1.4. References .................................................................................. 60 2. ROLE OF NATURAL NANOPARTICLES IN PHOSPHORUS TRANSPORT PROCESSES IN ULTISOLS ....................................... 85 2.1. Abstract ...................................................................................... 85 2.2. Introduction ................................................................................ 86 2.3. Materials and Methods ............................................................... 89 2.4. Results and Discussion .............................................................. 96 2.5. References ................................................................................ 109 viii Table of Contents (Continued) Page 3. REACTION CONDITIONS CONTROL SOIL COLLOID FACILITATED PHOSPHORUS RELEASE IN AGRICULTURAL ULTISOLS .................................................... 127 3.1. Abstract .................................................................................... 127 3.2. Introduction .............................................................................. 128 3.3. Materials and Methods ............................................................
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