Kinetics and Equilibrium of Barium and Strontium Sulfate Formation in Marcellus Shale Flowback Water
Publication: Journal of Environmental Engineering
Volume 140, Issue 5
Abstract
Flowback water from natural gas extraction in Marcellus Shale contains very high concentrations of inorganic salts and organic chemicals. Potential reuse of this water in subsequent hydraulic-fracturing operations may be limited by high concentrations of divalent cations (e.g., Ba, Sr, and Ca). Kinetics of barite and celestite precipitation in flowback waters from different well sites was evaluated in this study. Ba reacted rapidly with sulfate and reached equilibrium within 30 min, whereas Sr reacted slowly and took days to reach equilibrium. Equilibrium concentrations of Ba and Sr predicted by thermodynamics models were compared with experimental results. Activity corrections based on the Pitzer equation provided the best agreement with experimental data for both Ba and Sr. Comparison of barite and celestite precipitation kinetics in actual and synthetic flowback water revealed that there was no observable impact of organics and other minor components in actual flowback water on barite precipitation rate. This was primarily due to the fact that barite precipitation occurred relatively quickly at the high saturation levels utilized in this study. By contrast, lattice poisoning and complexation with organic matter had a profound impact on the comparatively slower celestite precipitation. The presence of organic matter in actual flowback water increased Ba and Sr concentrations in solution, and contributed to the discrepancy between measured and predicted equilibrium concentrations.
Get full access to this article
View all available purchase options and get full access to this article.
References
Agilent Technologies. (2010). Flame atomic absorption spectrometry: Analytical method, 10th Ed., Agilent Technologies, Santa Clara, CA.
Aniceto, J. P., Cardoso, S. P., Faria, T. L., Lito, P. F., and Silva, C. M. (2012). “Modeling ion exchange equilibrium: Analysis of exchanger phase non-ideality.” Desalination, 290(30), 43–53.
Barbot, E., Vidic, N., Gregory, K., and Vidic, R. D. (2013). “Spatial and temporal correlation of water quality parameters of produced waters from Devonian-age shale following hydraulic fracturing.” Environ. Sci. Technol., 47(6), 2562–2569.
Burkin, A. R. (2001). Chemical hydrometallurgy: Theory and principles, Imperial College Press, London, U.K.
Church, T. M., and Wolgemuth, K. (1972). “Marine barite saturation.” Earth Planet Sci Lett., 15(1), 35–44.
Davis, C. W. (1962). Ion association, Butterworths, London.
de Witt, W. (1993). “Principal oil and gas plays in the Appalachian basin (Province 131).” U.S. Geological Survey Bulletin 1839-I, U.S. Geological Survey, Washington, DC.
Economides, M. J., Watters, L. T., and Dunn-Norman, S. (1998). Petroleum well construction, John Wiley & Sons, West Sussex, England.
Engelder, T., and Lash, G. G. (2008). “Marcellus shale play’s vast resource potential creating stir in Appalachia.” Am. Oil Gas Reporter, 51(6), 76–87.
EPA. (1974). “Methods for the chemical analysis of water and wastes.”, U.S. Environmental Protection Agency, Washington, DC.
Fan, C., Kan, A. T., Zhang, P., and Tomson, M. B. (2011). “Barite nucleation and inhibition at 0 to 200°C with and without thermodynamic hydrate inhibitors.” SPE J., 16(2), 440–450.
Greenberg, J. P., and Moller, N. (1989). “The prediction of mineral solubilities in natural water: A chemical equilibrium model for the system to high concentrations from 0 to 250°C.” Geochim. Cosmochim. Acta, 53(10), 2,503–2,518.
Hamdona, S. K., Hamza, S. M., and Mangood, A. H. (2010). “The influence of polyphosphonates on the precipitation of strontium sulfate (celestite) from aqueous solutions.” Desalination Water Treat., 24(1–3), 55–60.
Harper, J. A. (2008). “The Marcellus shale: An old new gas reservoir in Pennsylvania.” Penn. Geol., 38(1), 2–13.
Harvie, C. E., Moller, N., and Weare, J. H. (1984). “The prediction of mineral solubilities in natural waters: The system to high ionic strength at 25°C.” Geochim. Cosmochim. Acta, 48(4), 723–751.
He, S., Oddo, J. E., and Tomson, M. B. (1995a). “The nucleation kinetics of barium sulfate in NaCl solutions up to 6 M and 90°C.” J. Colloid Interface Sci., 174(2), 319–326.
He, S., Oddo, J. E., and Tomson, M. B. (1995b). “The nucleation kinetics of strontium sulfate in NaCl solutions up to 6 M and 90°C with or without inhibitors.” J. Colloid Interface Sci., 174(2), 327–335.
Hennesy, A. J. B., and Graham, G. M. (2002). “The effect of additives on the co-crystallisation of calcium with barium sulfate.” J. Cryst. Growth, 237–239(3), 2153–2159.
Hill, D. G., Lombardi, T. E., and Martin, J. P. (2004). “Fractured shale gas potential in New York.” Northeastern Geol. Environ. Sci., 26(1/2), 57–78.
Holmes, H. F., Baes, C. F. B., Jr., and Mesmer, R. E. (1987). “The enthalpy of dilution of HCl(aq) to 648 K and 40 MPa: Thermodynamic properties.” J. Chem. Therm., 19(8), 863–890.
Jones, F., Oliviera, A., Parkinson, G. M., Rohl, A. L., Stanley, A., and Upson, T. (2004). “The effect of calcium ions on the precipitation of barium sulfate 1: Calcium ions in the absence of organic additives.” J. Cryst. Growth, 262(1–4), 572–580.
Jones, F., Piana, S., and Gale, J. D. (2008). “Understanding the kinetics of barium sulfate precipitation from water and water-methanol solutions.” Cryst. Growth Des., 8(3), 817–822.
Merkel, B. J., and Planer-Friedrich, B. (2008). Groundwater geochemistry: A practical guide to modeling of natural and contaminated aquatic systems, 2nd Ed., Springer-Verlag, Berlin.
Milici, R. C., and Swezey, C. S. (2006). Assessment of Appalachian basin oil and gas resources: Devonian Shale–middle and upper Paleozoic total petroleum system, U.S. Department of the Interior, U.S. Geological Survey, Reston, VA.
Miller, C. W., and Benson, L. V. (1983). “Simulation of solute transport in a chemically reactive heterogeneous system: Model development and application.” Water Resour. Res., 19(2), 381–391.
Monnin, C. (1999). “A thermodynamic model for the solubility of barite and celestite in electrolyte solutions and seawater to 200°C and to 1 kbar.” Chem. Geol., 153(1), 187–209.
Monnin, C., and Galinier, C. (1988). “The solubility of celestite and barite in electrolyte solutions and natural waters at 25°C: A thermodynamic study.” Chem. Geol., 71(4), 283–296.
Pabalan, R. T., and Pitzer, K. S. (1987). “Thermodynamics of concentrated electrolyte mixtures and the prediction of mineral solubilities to high temperatures for mixtures in the system .” Geochim. Cosmochim. Acta, 51(9), 2429–2443.
Parkhurst, D. L., and Appelo, C. A. J. (1999). “User’s guide to PHREEQC (version 2): A computer program for speciation, batch-reaction, one-dimensional transport, and inverse geochemical calculations.” U.S. Geological Survey, Water Resources Investigations Rep., 99-4259, Washington, DC.
Parkhurst, D. L., Thorstenson, D. C., and Plummer, L. N. (1980). “PHREEQE: A computer program for geochemical calculations.” U.S. Geological Survey, Water Resources Investigations Rep., 80-96, Washington, DC.
Pina, C. M., and Putnis, A. (2002). “The kinetics of nucleation of solid solutions from aqueous solutions: A new model for calculating non-equilibrium distribution coefficients.” Geochim. Cosmochim. Acta, 66(2), 185–192.
Pitzer, K. S. (1973). “Thermodynamics of electrolytes. I Theoretical basis and general equations.” J. Phys. Chem., 77(2), 268–277.
Pitzer, K. S. (1975). “Thermodynamics of electrolytes. V. Effects of higher-order electrostatic terms.” J. Solution Chem., 4(3), 249–265.
Pitzer, K. S. (1991). Activity coefficients in electrolyte solutions, 2nd Ed., CRC, Boca Raton, FL.
Pitzer, K. S., and Kim, J. J. (1974). “Thermodynamics of electrolytes. IV. Activity and osmosis coefficients for mixed electrolytes.” J. Am. Chem. Soc., 96(18), 5701–5707.
Pitzer, K. S., and Mayorga, G. (1973). “Thermodynamics of electrolytes. II. Activity and osmotic coefficients for strong electrolytes with one or both ions univalent.” J. Phys. Chem., 77(19), 2300–2308.
Pletcher, J. (2008). “Drillers access mile-deep gas deposits in what may be new ‘gold rush’.” Herald Standard, Uniontown, PA.
Risthaus, P., Bosbach, D., Becker, U., and Putnis, A. (2001). “Barite scale formation and dissolution at high ionic strength studied with atomic force microscopy.” Colloid. Surface Physicochem. Eng. Aspect., 191(3), 201–214.
Rodgers, M., et al. (2008). “Marcellus shale: What local government officials need to know.” Penn State Extension, College of Agricultural Sciences, Marcellus Education, University Park, PA.
Shen, D., Fu, G., Al-Saiari, H. A., Kan, A. T., and Tomson, M. B. (2009). “Barite dissolution/ precipitation kinetics in porous media and in the presence and absence of a common scale inhibitor.” SPE J., 14(3), 462–471.
Shen, D., Fu, G., Kan, H. A., and Tomson, M. B. (2008). “Seawater injection, inhibitor transport, rock-brine interactions, and scale control during seawater injection.” SPE Int. Oilfield Scale Conf., Society of Petroleum Engineers, Richardson, TX.
Smith, E., Hamilton-Taylor, J., William, D., Fullwood, N. J., and McGrath, M. (2004). “The effect of humic substances on barite precipitation-dissolution behaviour in natural and synthetic lake waters.” Chem. Geol., 207(1–2), 81–89.
Truesdell, A. H., and Jones, B. F. (1974). “WATEQ, a computer program for calculating chemical equilibria of natural waters.” J. Res. US Geol. Sur., 2(2), 233–274.
Van der Leeden, M. C. (1991). “The role of polyelectrolytes in barium sulfate precipitation.” Ph.D. dissertation, Technical Univ. of Delft, Delft, The Netherlands.
Vidic, R. D., Brantley, S. L., Vandenbossche, J. M., Yoxtheimer, D., and Abad, J. D. (2013). “Impact of shale gas development on regional water quality” Science, 340(6134), 1235009.
Westall, J. C., Zachary, J. L., and Morei, F. M. (1976). “MINEQL: A computer program for the calculation of chemical equilibrium composition of aqueous systems.”, Ralph M. Parsons Laboratory, Massachusetts Institute of Technology, Cambridge, MA.
Yeboah, Y. D., Saeed, M. R., and Lee, A. K. K. (1994). “Kinetics of strontium sulfate precipitation from aqueous electrolyte solutions.” J. Cryst. Growth, 135(1–2), 323–330.
Information & Authors
Information
Published In
Journal of Environmental Engineering
Volume 140 • Issue 5 • May 2014
Copyright
© 2014 American Society of Civil Engineers.
History
Received: Feb 22, 2013
Accepted: Nov 14, 2013
Published online: Jan 10, 2014
Published in print: May 1, 2014
Discussion open until: Jun 10, 2014
Authors
Metrics & Citations
Metrics
Citations
Download citation
If you have the appropriate software installed, you can download article citation data to the citation manager of your choice. Simply select your manager software from the list below and click Download.