Increased proliferation of nanotechnology has led to concerns regarding its implication to the water environment. Gold nanoparticles (AuNP) were used as a model nanomaterial to investigate the fate and dynamics of nanoparticles in the complex water environment. A column study was performed to examine the fate and transport of gold nanoparticles with two different coatings in porous media. The resulting data suggested that gold nanoparticles aggregate significantly in the porespace of the column interior, a finding that is not predicted by traditional colloidal filtration theory or Derjaguin-Landau-Verwey-Overbeek (DLVO) theory. Surface-enhanced Raman spectroscopy (SERS) was developed as a new technique to investigate AuNP aggregation in water with varying salt levels. The SERS technique proved valuable as an analytical technique, elucidating information about aggregation as well as AuNP surface interactions with dissolved halides in water. A thorough investigation examining Aunt aggregation with monovalent and divalent salts utilizing SERS, ultraviolet-visible light (UV-Vis) spectroscopy, and dynamic light scattering (DLS) was conducted. Each technique provided data describing different aspects of the dynamic behavior of AuNPs in complex water environments. Results suggest that in addition to attractive and repulsive interactions described by DLVO theory, chemical interactions between the AuNP surface and dissolved halides were also a significant driving force for aggregation and other transformative behaviors of AuNPs in water. The SERS technique developed in this work was shown to be a viable tool to help unveil the vastly complex dynamics of nanomaterial in the water environment. / Ph. D. / Nanotechnology is everywhere. It is in our smartphones, in our food, in our clothes, even if we do not recognize it is there. And this is a good thing, because nanotechnology – that is, technology that utilizes nanomaterials – can provide things that traditional technology often cannot. This is all because many nanomaterials have “superpowers” due to their size range: they are generally larger than what we may think of when we think of chemical molecules, but much smaller than macroscopic materials whose behaviors can be approximated by classic physics and chemistry. For example, we all know that gold has a shiny yellow metallic appearance. However, if we make little particles of gold – and these are going to be very tiny, with diameters about 10,000 times smaller than that of a strand of human hair (but about 100 times larger than what we would typically think of as molecules of chemicals) – and put them in water, the resulting mixture will be ruby-red like wine. One of the “superpowers” these gold nanoparticles possess is that they interact with light in a very different way than bulk gold. Currently, researchers in the biomedical field are producing promising work employing these particles in nextgeneration imaging, and much more. In this study, we were interested in what happens to these materials once they are released to the water environment. Because of the “superpowers” these gold nanoparticles possess, we really do not know how they will behave once they are released to either surface or groundwater because the physics and chemistry of those environments can be quite variable and complex. In this work, we have shown that traditional assumptions about particulate contaminants in water systems do not necessarily hold for gold nanoparticles. Laboratory simulations show that interactions between these particles and the surrounding environment that were once thought to be negligible, are in fact highly significant. As our title suggests, we are developing new and advanced “photonics” methods to help us discover the dynamic complexity dictating the fate of these gold nanoparticles once they are in the water environment. Photonics methods are techniques that employ light as a probing tool. These techniques use a well understood laser light source that is directed towards the particles in a water environment, and we then measure changes in the scattered light after it has interacted with the particles. The technique we have employed here (called surface-enhanced Raman spectroscopy, or SERS) simultaneously provides us information about different behaviors of gold nanoparticles in water, including how they may aggregate (that is, stick to one another and form big clumps) and how they interact with existing dissolved chemicals that may be present in the natural water environment. By pairing this method with other existing methods, we were able to paint a more complete picture of how these nanoparticles behave in the water environment, and we can answer some questions as to why they do not follow some previously held assumptions. In the end, the work in this dissertation will help future scientists continue to unlock the complexity of nanomaterial fate and dynamics in the water environment.
| Identifer | oai:union.ndltd.org:VTETD/oai:vtechworks.lib.vt.edu:10919/85437 |
| Date | 27 April 2017 |
| Creators | Chan, Matthew Yunho |
| Contributors | Civil and Environmental Engineering, Vikesland, Peter J., Marr, Linsey C., Pruden, Amy, Hochella, Michael F. Jr. |
| Publisher | Virginia Tech |
| Source Sets | Virginia Tech Theses and Dissertation |
| Detected Language | English |
| Type | Dissertation |
| Format | ETD, application/pdf |
| Rights | In Copyright, http://rightsstatements.org/vocab/InC/1.0/ |
Page generated in 0.0038 seconds