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Fate and Transport of Nanoscale Buckminsterfullerene Aggregates (Nc60) in Heterogenous Porous Media

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Fate and Transport of Nanoscale Buckminsterfullerene Aggregates (Nc60) in Heterogenous Porous Media Fate and Transport of Nanoscale Buckminsterfullerene Aggregates (nC60) in Heterogenous Porous Media An Honors Thesis for the Department of Civil and Environmental Engineering Committee Members: Dr. Kurt Pennell, Dr. C. Andrew Ramsburg, Dr. Linda Abriola Jordyn Wolfand Tufts University May 6, 2011 ABSTRACT Buckminsterfullerene (C60), an allotrope of carbon, has unique physical and chemical properties that have led to its use in a variety of commercial applications, ranging from organic photovoltaics to biopharmaceuticals. It is inevitable that C60 will be released into the environment during manufacture, transportation, application, and disposal. C60 is nearly insoluble in water, though several methods have been developed to disperse C60 aggregates in water without the aid of stabilizing agents. These C60 aggregates have diameters of 5–200 nm, are negatively charged, and are referred to as nC60. It has been suggested that nC60 is the most environmentally relevant form of C60, but understanding of the retention and transport of these particles in heterogeneous is limited. This research sought to characterize the transport and retention behavior of nC60 in a two-dimensional (2-d) aquifer cell packed with heterogeneous porous media. It was hypothesized that nC60 would accumulate at the interfaces between high and low permeability sands. Initially, two sets of one-dimensional (1-d) column experiments were completed to prepare for injection into the 2-d aquifer cell, and to determine parameters needed to simulate transport of nC60 with modified filtration theory. The first series of column studies was conducted to determine a background electrolyte that would result in 75% breakthrough of nC60 after a pulse injection into the 40/50 mesh sand matrix. A second series of 1-d column experiments was completed at the optimal electrolyte concentration to determine two parameters needed for simulation by modified filtration theory—maximum retention capacity (Smax), and the particle attachment rate (Katt) of the porous medium. After determination of the relevant transport parameters in the 1-d column studies, nC60 was injected into the 2-d aquifer cell. nC60 breakthrough was found to increase with an increase in ionic strength of the background electrolyte, in accordance with previous literature. 6 mM NaCl and 0.05 mM NaHCO3 was chosen as the background electrolyte for the 2-d cell. Smax was determined to be 0.57, 3.17, and -1 0.54, 3.2, and 4.7 μg/g, and katt was found to be 0.25, 1.1, and 1.4 h for 40/50, 80/100, and 100/140 mesh natural Ottawa sand, respectively. nC60 was injected separately into three of the ports of the 2-d aquifer cell (upstream of a 80/100 mesh low-permeability lens, upstream of a 100/140 mesh low-permeability lens, and in the background matrix of 40/50 mesh sand. A significant amount of nC60 mass was retained near the port of injection. Enhanced accumulation of sorbed-phase nC60 at the textural interface did not occur as expected. Though sorbed-phase concentration of nC60 decreased after the interface, accumulation did not occur on the horizontal boundaries of the lens. Results indicate that nC60 transport at textural interfaces is controlled by changes in local flow velocities through heterogeneous media. ii TABLE OF CONTENTS Abstract ii Table of Contents iii List of Acronyms and Initialisms iv List of Symbols vi List of Figures viii List of Tables xi 1.0 Introduction 1 2.0 Literature Review 1 2.1 Properties and Applications of C60 1 2.2 Dispersion of C60 in Water 2 2.3 Toxicity of nC60 3 2.4 Fate and Transport of nC60 4 3.0 Purpose 8 4.0 Hypothesis 10 5.0 Materials and Methods 12 5.1 nC60 Preparation and Characterization 12 5.2 One-Dimensional Column Studies 14 5.2.1 1-D column set-up 15 5.2.2 Effect of background electrolyte on nC60 transport 18 5.2.3 Effect of soil particle size on nC60 transport 19 5.3 Two-Dimensional Aquifer Cell 20 5.3.1 2-D aquifer cell set-up 20 5.3.2 Non-reactive tracer tests 23 5.3.3 nC60 injection 24 5.4 Quantification of Aqueous nC60 26 5.4.1 Quantification by UV-VIS 26 5.4.2 Quantification by HPLC 28 5.5 Quantification of Solid-phase nC60 31 6.0 Results and Discussion 32 iii 6.1 1-D Column Studies 32 6.1.1 Effect of background electrolyte on nC60 transport 32 6.1.2 Effect of soil particle size on nC60 transport 34 6.2 2-D Aquifer Cell 41 6.2.1 Non-reactive breakthrough tracer tests 41 6.2.2 nC60 injection 45 7.0 Conclusions and Recommendations 54 8.0 Collaboration and Acknowledgements 56 List of References 57 iv LIST OF ACRONYMS AND INITIALISMS ADR Advective-dispersive reaction BTC Breakthrough tracer curve CaBr2 Calcium bromide CaCl2 Calcium chloride C60 Buckminsterfullerene (Carbon-60) DLS Dynamic light scattering DSLR Digital single-lense reflex DVLO Derjaguin-Landau-Verwey-Overbeek HPLC High performance liquid chromatography IC Ion chromatography LC50 Median lethal dose NaCl Sodium chloride NaFlour Sodium flourescein nC60 Nano-scale buckminsterfullerene aggregates PV Pore volume THF Tetrahydrofuran UV-VIS Ultraviolet-visible spectrophotometry v LIST OF SYMBOLS α attachment efficiency factor αL longitudinal dispersivity coefficient αT transverse dispersivity coefficient C concentration in the effluent aqueous phase C0 concentration in the influent aqueous phase dc mean diameter of the porous medium d50 Mass-median-diameter DL longitudinal hydrodynamic dispersion coefficient * DL longitudinal molecular diffusion coefficient η0 theoretical clean-bed single collector efficiency g acceleration of gravity λ wavelength K permeability katt particle attachment rate ki intrinsic permeability L characteristic length μ viscosity of water n porosity ρ density of water ρb soil bulk density Pe Péclet number S concentration in the solid-phase vi Smax maximum retention capacity t time θw volumetric water content vp pore-water velocity vii LIST OF FIGURES Figure 1. The molecular structure of C60 2 Figure 2. Mechanisms for colloid attachment according to classical filtration theory 5 Figure 3. Illustration of strained colloids in the smallest regions of the soil pore space 7 Figure 4. Side-view of 2-d aquifer cell with low permeability lenses 9 Figure 5. Comparison of Smax as functions of sand grain size at two velocities 10 Figure 6. Vector maps for velocity flow for fully screened influent at left inlet and injection into ports A2 and A4 11 Figure 7. Preliminary modeling results 12 Figure 8. Sample outputs from DLS for particle size and zeta potential of nC60 14 Figure 9. 1-d column apparatus 15 Figure 10. Representative bromide standard curve 16 Figure 11. Column experiment apparatus and set-up 18 Figure 12. Dimensions of the 2-d aquifer cell and sampling ports 22 Figure 13. 2-d aquifer cell set-up 22 Figure 14. Schematic of nC60 injections into the 2-d aquifer cell 25 Figure 15. Grid of box-sections to determine sorbed-phase concentration distribution after nC60 injection 25 Figure 16. Representative standard curve for aqueous nC60 detection by UV-VIS 27 Figure 17. UV-VIS sample output for absorbance of nC60 28 Figure 18. Representative standard curve for nC60 detection by HPLC 29 Figure 19. Sample chromatogram from HPLC 30 Figure 20. Hubaux-Vos graph to determine the detection limit of C60 by HPLC 31 Figure 21. nC60 breakthrough curves in 40/50 mesh OS with various background electrolytes 33 viii Figure 22. Breakthrough curve and retention profile for nC60 injection into 40/50 OS 35 Figure 23. Breakthrough curve and retention profile for nC60 injection into 80/100 OS 36 Figure 24. Breakthrough curve and retention profile for nC60 injection into 100/140 OS 37 Figure 25. Non-reactive tracer data in 40/50 mesh OS fit to the 1-d equilibrium ADR transport equation 38 Figure 26. Non-reactive tracer data in 80/100 mesh OS fit to the 1-d equilibrium ADR transport equation 39 Figure 27. Non-reactive tracer data in 100/140 mesh OS fit to the 1-d equilibrium ADR transport equation 39 Figure 28. Modified filtration theory fit to experimental breakthrough curves for various sand particle sizes 40 Figure 29. Photograph of non-reactive sodium flourescein and sodium bromide tracer through fully screened influent chamber 42 Figure 30. BTCs for fully-screened non-reactive tracer in 2-d cell fit for dispersivity coefficients 43 Figure 31. Time-series photographs of sodium flourescein injection through port A2 44 Figure 32. Time-series photographs of sodium flourescein injection through port A4 45 Figure 33. Photographs of influent ports after nC60 injection 46 Figure 34. Photograph of nC60 injection solution 47 Figure 35. Plot of solid-phase concentration of nC60 around injection port A4 48 Figure 36. Plot of solid-phase nC60 concentration around the 100/140 mesh lens 48 Figure 37. nC60 retained immediately before the 40/50 and 100/140 mesh interface 49 Figure 38. nC60 retained immediately after the 40/50 and 100/140 mesh interface 49 Figure 39. Retention profiles for horizontal transects outside of 100/140 mesh lens 50 ix Figure 40. Retention profiles for horizontal transects through the 100/140 mesh lens 50 Figure 41. Plot of solid-phase nC60 concentrations in the background matrix 51 Figure 42. Comparison of nC60 retention profiles 52 Figure 43. Scaled comparison of nC60 retention profiles 52 Figure 44. Comparison of retention profiles in the column and aquifer cell 53 x LIST OF TABLES Table 1. Experimental conditions for the first set of column experiments 19 Table 2. Experimental conditions for the second set of column experiments 20 Table 3.
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