Dissolution and Heavy Residue Sinking of Subsurface Oil Droplets: Binary Component Mixture Dissolution Theory and Model-Oil Experiments
Publication: Journal of Environmental Engineering
Volume 143, Issue 10
Abstract
The processes by which oil-material appears suspended in the water column or becomes deposited on the sea floor is conventionally attributed to its attachment to marine solid particles. Since the 2010 Gulf oil spill, a significant volume has remained unaccounted for. The fraction volume of oil sinking resulting from dissolution of its lighter components is the subject of this work. An experimental study and theoretical development for the combined processes of oil-droplet dissolution/sinking (named SOLUTE-SINK) is based on a conceptual binary-component model for crude oil. The experiments were on buoyant pseudo-oils, a two-component (A and B) miscible hydrocarbon mixture formulated from a less-dense-than-water liquid hydrocarbon (Component A) and a more-dense-than-water hydrocarbon-like chemical (Component B). These were used in proof-of-concept experiments. A single, buoyant liquid drop surrounded by water was constrained from floating to the surface in a laboratory-scale microcosm dissolution tank. It was placed inside an inverted and submerged Petri dish so evaporation was not possible and weathering occurred by dissolution only. The heavier-than-water Component B was much less soluble; during the experiment, Component-A dissolution losses resulted in droplet sinking. This established proof-of-concept and the observed time period provided key data supporting the proposed oil binary-model theory. Experiments were performed with four binary chemical mixtures, each replicated 5–7 times. The dissolution time periods for achieving buoyancy inversion (i.e., sinking droplet) ranged from 2 to 4 days with the kinetics parameter dependent on the solubility of Component A. Concentration and bulk density measurements tracked the theoretical time-series behavior of the proposed model equations. Direct mathematical coupling the dissolution/buoyancy loss process for single liquid droplet in the water column is an original contribution of this work. In knowing the initial drop-size distribution, the field of oil-spill modeling is provided with an algorithm forecasting four oil-material produced fractions: dissolved, floating, suspended, and sinking. The SOLUTE-SINK model will find applications for deep-water blowout ejected droplets (constrained to dissolution weathering only) as well as breaking-wave-produced droplets for sea surface spills. In addition, it will aid the development of a laboratory method for the oil dissolution process.
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Acknowledgments
The Cain Department of Chemical Engineering, Gulf of Mexico Research Institute (GOMRI) and National Oceanic Atmospheric Administration (NOAA) provided all financial resources for the work. Several undergraduate students provided valuable service doing experiments, reviewing the literature, making computations, etc., and they include Seth Brown, David Galin, Ta’Ryan Lloyd, Ryan Ledoux, Steven Nguyen, and Jose Alves Da Cruz Junior. The manuscript is dedicated to LSU student David James Galin, who lost his life tragically.
References
Almeda, R., Hyatt, C., and Buskey, E. J. (2014). “Toxicity of dispersant Coreit 9500A and crude oil in microzooplankton.” Ecotoxicol. Environ. Saf., 106, 76–85.
Aman, Z. M., Haber, A., Ling, N. N. A., Thornton, A., Johns, M. L., and May, E. F. (2015). “Effect of brine salinity on the stability of hydrate-in-oil dispersion and water-in-oil emulsions.” Energy Fuels, 29(12), 7948–7955.
Anderson, S. E., Franko, J., Lukomska, E., and Meade, B. J. (2011). “Potential immunotoxicological health effects following exposure to COREXIT 9500A during cleanup of the Deepwater Horizon oil spill.” J. Toxicol. Environ. Health, Part A, 74(21), 1419–1430.
Blanchard, D. C. (1975). “Bubble scavenging and air-to-water transfer of organic material in the sea.” Appl. Chem. Protein Interf., 145, 306–387.
Boehm, P., Flest, D., MacKay, D., and Paterson, S. (1982). “Physical-chemical weathering of petroleum hydrocarbons from the IXTOC I blowout: Chemical measurements and a weathering model.” Environ. Sci. Technol., 16(8), 495.
Brookman, G. T., and Flanagan, M. (1985). “Laboratory study on solubilities of petroleum hydrocarbons in groundwater.”, American Petroleum Institute, Washington, DC.
Brown, J. S., Beckmann, D., Bruce, D., and Mudge, S. (2011). “PAH depletion ratios document the rapid weathering and attenuation of PAHs in oil samples collected after the DWH incident.” Proc., 2011 Oil Spill Conf., Portland, OR.
Campo, P., Venosa, A. D., and Sudian, M. T. (2013). “Biodegradability of Corexit 9500 and dispersed south Louisiana crude oil.” Environ. Sci. Technol., 47(4), 1960–1967.
Cohen, Y. (1983). “Mass transfer across a sheared, wavy air-water interface.” Int. J. Heat Mass Transfer, 26(9), 1289–1297.
Cohen, Y., Cocchoio, W., and Mackay, D. (1978). “Laboratory studies of liquid-phase controlled volatilization rates in the presence of wind waves.” Environ. Sci. Technol., 12(5), 553–558.
Daling, P. S., et al. (2014). “Surface weathering and dispersability of MC 252 crude oil.” Mar. Pollut. Bull., 87(1), 300–310.
Ehrenhauser, F. S., et al. (2014). “Bubble bursting as an aerosol generation mechanism during an oil spill in the deep environment: Laboratory experimental demonstration of the transport pathway.” Environ. Sci. Processes Impacts 16(1), 65–73.
French, D., Schuttenberg, H., and Isaji, T. (1999). “Probabilities of oil exceeding thresholds of concern: Examples from an evaluation for Florida Power and Light.” Proc., 22nd Arctic and Marine Oil Spill Program (AMOP) Technical Seminar, Calgary, AL, Canada, 243–270.
French-McCay, D. P. (2004). “Oil spill impact modeling: Development and validation.” Environ. Toxicol. Chem., 23(10), 2441–2456.
Gros, J., Reddy, C. M., Nelson, R. K., Socolofsky, S. A., and Arey, J. S. (2016). “Simulating gas-liquid-water partitioning and fluid properties of petroleum under pressure: Implications for deep sea blowouts.” Environ. Sci. Technol., 50(14), 7397–7408.
Gulliver, J. S. (2011). “Air–water mass-transfer coefficients.” Handbook of chemical mass transport in the environment, L. J. Thibodeaux and D. MacKay, eds., CRC Press, Boca Raton, FL.
Habartova, A., Valsaraj, K. T., and Roselova, M. (2013). “Molecular dynamics simulations of small halogenated organics, at the air/water interface: Implications in water treatment and atmospheric chemistry.” J. Phys. Chem. A, 117(38), 9205–9215.
Hamam, S., Hamoda, M., Shaban, H., and Kilani, A. (1987). “Crude oil dissolution in saline water.” Water Air Soil Pollut., 37(1), 55–64.
Hornbeck, R. W. (1975). Numerical methods, Quantum, New York.
Jernelov, A. (2010). “The threats from oil spills: Now, then and in the future.” AMBIO, 39, 353–366.
Johansen, O. H., Brandvik, P. J., and Farooq, U. (2013). “Droplet breakup in subsea release. II: Prediction of the droplet size distribution with and without injection of chemical dispersants.” Mar. Pollut. Bull., 73(1), 327–335.
Johansen, O. H., Rye, H., and Cooper, C. (2003). “Deep spill-field study of a simulated oil and gas blowout in deep water.” Spill Sci. Technol. Bull., 8(5), 433–443.
Joye, S., MacDonald, I. R., Leifer, I., and Asper, V. (2011). “Magnitude and oxidation potential of hydrocarbon gases released from the BP oil well blowout.” Nature Geosci., 4(3), 160–164.
Kilpatrick, P. K., and Spiecker, P. M. (2001). “Asphaltene emissions.” Encyclopedic handbook of emulsion technology, J., Sjoblom, ed., Marcel Dekker, New York.
King, T. L., Robinson, B., Boufadel, M., and Lee, K. (2014). “Flume-tank studies to elucidate the fate and behavior of diluted bitumen spilled at sea.” Mar. Pollut. Bull., 83(1), 32–37.
Lee, L. S., Hagwall, M., Delfino, J. J., and Rao, P. S. C. (1992). “Partitioning of polycyclic aromatic hydrocarbons from diesel fuel into water.” Environ. Sci. Technol., 26(11), 2104–2110.
Lehr, W. J., Jones, R., Evans, M., Simecek-Beatty, D., and Overstreet, R. (2002). “Revisions of the ADIOS oil spill model.” Environ. Model. Software, 17(2), 191–199.
Levitt, D. (2010). “Quantitative relationship between the octanol/water partition coefficient and the diffusion limitation of the exchange between adipose and blood.” BMC Clin. Pharmocol., 10(1), 1–13.
Liyana-Arachchi, T. P., Zhang, Z., Ehrenhauser, F. S., Avij, P., Valsaraj, K. T., and Hung, F. R. (2014). “Bubble bursting as an aerosol generation mechanism during an oil spill in the deep-sea environment: Molecular dynamic simulations of oil alkanes and dispersants in the atmospheric air/salt water interfaces.” Environ. Sci. Processes Impact, 16(1), 53–64.
Loebig, C. J. (2015). “Sinking of crude oil amended-model oil mixtures due to evaporation and dissolution weathering: Spill simulation experiments and scale-up models.” Master thesis, Louisiana State Univ., Baton Rouge, LA, 45.
Loh, A., Shim, W. J., Yong, S., and Yim, H. U. H. (2014). “Oil-suspended particulate matter aggregates: Formation mechanism and fate in the marine environment.” Ocean Sci. J., 49(4), 329.
Mackay, D., Buist, I., Mascarenhas, R., and Paterson, S. (1980a). “Oil spill processes and models.”, Environment Canada, Ottawa.
Mackay, D., Paterson, S., and Trudel, K. (1980b). “A mathematical model of oil spill behavior.”, Environment Canada, Ottawa.
MacKay, D., and Yeun, A. (1983). “Mass transfer coefficient correlations for volatilization of organic solutes from water.” Environ. Sci. Technol., 17(4), 211–217.
McLean, J. D., and Kilpatrick, P. K. (1997). “Effects of asphaltene aggregation in model heptane-toluene mixtures on stability of water-in-oil emulsions.” J Colloid Interf. Sci., 196(1), 23–34.
Melvin, A. T., Thibodeaux, L. J., Parsons, A. R., Overton, E., Valsaraj, K. T., and Nandakumar, K. (2016). “Oil-material fractionation in Gulf deep water horizontal intrusion layer: Field data analysis and chemodynamic model fate model for Macondo 252 oil spill.” Mar. Pollut. Bull., 105(1), 110–119.
Mendelssohn, I. A., et al. (2012). “Oil impacts on coastal wetlands: Implications for the Mississippi River delta ecosystem after the Deepwater Horizon spill.” BioSciences, 62(6), 562–574.
Middlebrook, A. N., et al. (2011). “Air quality implications of the Deepwater Horizon oil spill.” ⟨www.pnas.org/cgi/⟩ (Jun. 22, 2011).
Mills, M. A., McDonald, T. J., Bonner, J. S., Simmons, M. A., and Autenreith, R. L. (1999). “Method of quantifying the fate of petroleum in the environment.” Chemosphere, 39(144), 2563–2582.
Muschenheim, D. K., and Lee, K. (2003). “Removal of oil from the sea surface through particulate interactions: Review and prospectus.” Spill Sci. Technol. Bull., 8(1), 9–18.
NRC (National Research Council). (1985). Oil in the sea: Inputs, fates, and effects, Washington, DC.
NRC (National Research Council). (2005). Oil spill dispersants: Efficacy and effects, Washington, DC.
Page, C. A., Bonner, J. S., Sumner, P. S., and Autenrieth, R. L. (2000). “Solubility of petroleum hydrocarbons in oil/water systems.” Mar. Chem., 70(1), 79–87.
Peterson, C. H., et al. (2012). “A tale of two spills: Novel science and policy implications of an emerging new oil spill model.” Biosciences, 62(5), 461–469.
Reddy, C., et al. (2011). “Composition and fate of gas and oil released to the water column during the Deepwater Horizon oil spill.” Proc. Natl. Acad. Sci. U.S.A., 109(50), 20229–20234.
Reed, M., et al. (1999). “Oil spill modeling towards the close of the 20th century: Overview of the state of the art.” Spill Sci. Technol. Bull., 5(1), 3–16.
Reinhard, M., and Drefahl, A. (1999). Handbook for estimating physicochemical properties of organic compounds, Wiley, New York.
Ryerson, T. B., et al. (2011). “Atmospheric emissions from the Deepwater Horizon spill constraint air-water partitioning, hydrocarbon fate, and leak rate.” Geophys. Res. Lett., 38 (7).
Sangster, J. (1997). Octanol water partition coefficients: Fundamentals and physical chemistry, Wiley, West Sussex, U.K., 157–167.
Scholz, D. K., et al. (1999). Fate of spilled oil in marine waters: Where does it go? What does it go? How do dispersants affect it?, Dept. of Health and Environmental Sciences, American Petroleum Institute, Washington, DC, 1–43.
Singh, S., McLean, J. D., and Kilpatrick, P. K. (1999). “Fused ring aromatic solvency in destabilizing water-in-asphaletne-heptane-toluene emulsions.” J. Dispersion Sci. Technol., 20(1–2), 279–293.
Socolofsky, S., Adams, E., and Sherwood, C. (2011). “Formation dynamics of subsurface hydrocarbon intrusions following the Deepwater Horizon blowout.” Geophys. Res. Lett., 38(9), L09602.
Solomon, G. M. (2010). “Health effect of the Gulf oil spill.” JAMA, 304(10), 1118.
Speight, J. (1991). The chemistry and technology of petroleum, Marcel Dekker, New York, 401–470.
Stevens, C. C. (2014). “Sinking of hydrocarbon mixtures due to the evaporative and/or dissolution weathering on the surface and submerged in water.” M.S. thesis, Louisiana State Univ., Middleton Library, Baton Rouge, LA.
Stevens, C. C., et al. (2015). “Sea surface oil slick light component vaporization and heavy residue sinking: Binary mixture theory and experimental proof of concept.” Environ. Eng. Sci., 32(8), 694–702.
Stiver, W., and Mackay, D. (1984). “Evaporation rate of spills of hydrocarbons and petroleum mixtures.” Environ. Sci. Tech., 18, 834–840.
Teal, J., and Howarth, R. (1984). “Oil spill studies: A review of ecological effects.” Environ. Manage., 8(1), 24–42.
Thibodeaux, L., Valsaraj, K., John, V., Papadopoulos, D., Pratt, L., and Pesika, N. (2011). “Marine oil fate: Knowledge gaps, basic research, and development needs: A perspective based on the Deepwater Horizon spill.” Environ. Eng. Sci., 28(2), 87–93.
Thibodeaux, L. J. (1996). Environmental chemodynamics, 2nd Ed., Wiley, New York, 264–269.
Venosa, A. D., Anastas, P. T., Barron, M. G., Conmy, R. N., Greenburg, M. S., and Wilson, G. T. (2014). “Science-based decision making on the use of dispersants in the Deepwater Horizon oil spill.” Oil spill remediation: Colloid chemistry-based principles and solutions, P. Patra, R. S. Farinato, and K. Papadoppulos, eds., 1st Ed., Wiley, New York, 1–17.
White, H. K., et al. (2012). “Impact of the Deepwater Horizon oil spill on a deep-water coral community in the Gulf of Mexico.” ⟨www.pnas.org/cgi/doi⟩ (Nov. 1, 2011).
Wise, C. F., Wise, J. T., Wise, S. S., Thompson, W. D., and Wise, J. P. (2014). “Chemical dispersants used in the Gulf of Mexico oil crisis are cytotoxic and genotoxic to sperm whale skin cells.” Aquat. Toxicol., 152, 335–340.
Zhao, L., et al. (2015). “Simulation of scenarios of oil droplet from Deepwater Horizon blowout.” Mar. Pollut. Bull., 102, 304–319.
Zhendi, W., et al. (2003). “Characteristics of spilled oils, fuels, and petroleum products. I: Composition and properties of selected oils.”, NERL, Triangle Park, NC, 280.
Zhoa, X., Gong, Y., O’Reilly, S., and Zhoa, D. (2015). “Effects of oil dispersants on solubilization, sorption and desorption of polycyclic aromatic hydrocarbons in sediment seawater systems.” Mar. Pollut. Bull., 92, 160–169.
Zock, J. P., et al. (2007). “Prolonged respiratory symptoms in clean-up workers of the Prestige oil spill.” Am. J. Respir. Crit. Care Med., 176, 610–616.
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Published In
Journal of Environmental Engineering
Volume 143 • Issue 10 • October 2017
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©2017 American Society of Civil Engineers.
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Received: Jun 28, 2016
Accepted: Feb 6, 2017
Published online: Jul 20, 2017
Published in print: Oct 1, 2017
Discussion open until: Dec 20, 2017
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