ODYSSEY ENABLED Call #: TP 1 .C36x ; Location: SCIENCE 2nd FLOOR 1(1973) TNH: 758180 460(1997) (73 . (ANIL isan Journal Title: Chemical engineering ‘communications. Article Author: Article Title: E-Mail: tev amin amt ed? Solubility in Conditions BZEOOLOZ Ariel Address: 12! 2 Volumelissue: Month/Year: 1990 8 8 2 8 ILL #: 69481996 iui WA Patron: Bustamante, Elizabeth M libraryexpresst 3 2 £ s a 6 € 9 a < Lending String: Notice: This material may be protected by Copyright Law (Title 17 U.S.C.Chem. Eng. Comm. 199, Vol. $0, pp. 23-33, Reprints available iret from the publisher. Photocopying permitted by license only {© 1980 Gordon and Breach Science Publishers 5.A. Printed inthe United States of America CO, SOLUBILITY IN WATER AND BRINE UNDER RESERVOIR CONDITIONS . ROBERT M. ENICK se Associated University Fellow University of Pitsburgh 1249 Benedum Engineering Hall Department of Chemical and Petroleum Engineering Pittsburgh, PA 15261 and SCOTT M. KLARA ‘Morgantown Energy Technology Center U.S. Department of Energy P.O. Box 880 Morgantown, WV 26507-0880 (Received November 7, 1988; im fnal form October 31, 1989) ‘The reference Henry's constant was determined from 110 solubility data found in the literature fr the CO,/H,O ‘system over a temperature range of 298 to 523K and a pressure range of 3.40 to ‘TAI MPa, Since the Krichevsky-linskaya equation was used to model the system, a correlation for the A parameter was ako developed. In adkltion to the. Krichevsky-llinskaya equation, another two-parameter correlation for the solubility of carbon dioxide in water was obtained by using the Krichevsky~Kasarmovsky equation. ‘The reference Henry's constant and partial molar volume of carbon dioxide at infinite dition were ‘teated as adjustable parameters. The calculated values ofthe partial molar volume at infinite dilation 4d not correspond 10 experimentally determined values found in the literature. Therefore, a thitd -eorrelation forthe reference Henrys constant was obtained by using the Krichevsky-Kasarnovsky ‘equation in conjunction with the correct values of the partial molar volume. This one parameter ‘(Henry's constant) model didnot tthe experimental data is wel as the two parameter models. "The deereased Solbilty of CO; in brine was acounted for empirically by a single factor corelated to the weight percent of dissolved solids. A literature dataset of 167 solubilities, with a temperature ‘ange of 298 to_523 K and a pressure range of 3.0 to 85.0MPa, was used to develop this correlation. A wie scatter of data characterizes this corelation, which relates the CO, solubility in brine to the COs solubility in water at the same temperature and pressure. The corelation is designed for applications in which the determination of concentrations of fndividual ions fs impractical and the implementation ‘of only one additional parameter is desirable, such as the se of compositional simulators to model miscible displacement inthe petroleum industry ‘These correlations can be easly implemented into reservoir simulation calculations to account for the effecs of CO, solubility in Brine. These effects ae often ignored even though they can have dramatic effets on the performance of the CO; enhanced oil recovery process. The correlations presented in this paper for the Henry's constant and the effect of dissolved solids can adequately account for these CO, solubility effec. ‘KEYWORDS Solubility Henry's constant Carbon dioside Brine High-pressure. zB4 ROBERT M. ENICK AND SCOTT M. KLARA INTRODUCTION Most carbon dioxide (CO,) miscible displacement phase behavior studies have concentrated on the CO,/hydrocarbon phase equilibria, even though brine exists naturally in the reservoir, is injected during the waterflood, and is also introduced into the formation along with CO; in order to inhibit its tendency to “finger” through the relatively viscous oil. The primary thermodynamic effect of the aqueous phase has been assumed to be its solubilization of light gases, especially CO;, since water and liquid hydrocarbons are relatively ible at reservoir conditions. Many investigators have proposed using Henry's law to model the gas solubility in pure water and an equation of state to describe the hydrocarbon phase equilibria. Several empirical correlations for the Henry's constant or reference Henry's constant of CO» in water have been published,” but that of Li and Nghiem® is ‘mote appropriate for reservoir conditions since it was based on high pressure data. The partial molar volume of CO, at infinite dilution in water, a parameter in the Poynting correction used in the Henry's law analysis, is often estimated using the correlation of Lyckman et ai.,” as reported in a simple correlation by Heidemann and Prausnitz.* Li and Nghiem® have suggested a modification of the Henry's constant to account for dissolved solids. Scaled particle theory (SPT) was used to account for the decreased solubility of light gases. The molecular diameter of the solute, a parameter that has a strong effect on SPT predictions, ‘was optimized to match the solubility of CO, in brine. Water solubility in the hydrocarbon phases, including the CO,-rich vapor or liquid, is typically neglected since it is very small over the range of reservoir conditions. However, this aspect can be incorporated into phase behavior Cubic equations of state have also been employed in an attempt to describe all fluid phases with one model.** Recently, Panagiotopolous and Reid! pre- sented a mixing rule for highly polar asymmetric systems such as CO,/H,O. Enick, Holder, and Mohamed" incorporated this mixing rule into a three/four- phase flash algorithm's and subsequently Pollack et al.,!° demonstrated its ability to predict the effect of an aqueous phase (water or brine) on CO,/hydrocarbon phase behavior. This same study, however, indicated that the results obtained by neglecting water solubility in the hydrocarbon phases and modeling CO; solubility in brine using Henry's law and an empirical factor to account for a decrease in solubility due to dissolved solids were very similar to those obtained from the equation-of-state. Both modeled the experimentally observed shift in the pressure-composition diagram of CO,/crude oil systems. Since Henry's law algorithm usually involves less computational time and trouble, it was considered to be the preferable alternative. ‘The purpose of this study, therefore, was to accurately correlate carbon dioxide solubility in water by regressing the Henry constant for the CO,/H,O system using all available literature data at reservoir conditions. The fugacity of CO, was calculated with the Peng-Robinson equation of state since that equation is. commonly used in compositional simulation. The effect of dissolved solids on theCO, SOLUBILITY IN WATER AND BRINE 25 solubility of CO, in the aqueous phase was also determiried by evaluating literature data at reservoir conditions. This effect was correlated to a single parameter, the total dissolved solids (TDS) concentration, since it not only is a commonly used parameter for brines, but also requires the use of only one additional material balance in a compositional simulator. CO, SOLUBILITY IN' WATER A large volume of data exists on the solubility of CO, in water." Many experimental studies have also been performed to determine the solubility of water in CO,.”27"=* Panagiotopolous and Reid" have correlated mutual solubility data in the 298 to 348K range, using the Peng-Robinson equation of state and a two parameter mixing rule for highly polar asymmetric systems. Their work was extended by Enick, Holder, and Mohamed" to 383K. Li and Nghiem® used Henry's law and an equation of state to describe the aqueous and COz-rich phases, respectively, over a 298 to 523 K temperature range and a 6.9 to 100 MPa pressure range. Approximately 60 CO, solubilities were used in their study. The partial molar volume of CO, at infinite ditution in water was estimated using the Lyckman et al., correlation’ as presented by Heidemann and Prausnitz.? The gas and liquid phase compositions were regressed by optimizing the gas phase raction parameter and the Henry's constant. In our study, 110 solubilities (consisting of all of the data from the aforemen- tioned CO,-solubility data base which fell within the temperature and pressure range of interest) along 12 isotherms between 298 and 523 K were compiled over a 3.40 to 72.41MPa pressure range. The data from all sources were used together, they were not treated separately. These data were used to find the value of the reference Henry's constant,® Héo,, which best satisfied the following ‘expression at each temperature. Since Seon _ 1; a Yeon then $005.) s00 Zo g « 200 00 | em xxi aspen J ema, tomt.7 f Li and Nghier® ol . ‘200 250 900-350 400 450 500 S50 600 Temperature (K) FIGURE 1 Correlations for the Henry constant of the CO,/H,0 system,CO, SOLUBILITY IN WATER AND BRINE, 2 * as 2 « S =z 3 as 20 ® Sahusttle prometer (| ‘20050 300350000500 680600 Temperature K) FIGURE 2. Correlations for the partial molar volume of carbon dioxide at infinite dilution in water. using Eq. (3) and the Lyckman et al.,” correlation since two parameters were adjusted to match the data rather than one. Parkinson and DeNevers" first noted that partial molar volumes obtained in this manner for the CO,/H,O system did not correspond to experimental values even though linear plots of Eq. (2) with high correlation coefficients were obtained. This is clearly evident in our results by the decrease in OZo, at high temperatures, Figure 2. This trend is contrary to experimentally determined values of 3Zo,,1"* which are well represented by the Lyckman et al.,” correlation over this temperature range. Gibbs and Van Ness“ explained that it was possible 10 correlate solubilities for the CO,/H,O system in this manner, but the partial ‘molar volumes at infinite dilution could bear no similarity to actual values. They showed that the Krichevsky-Hinskaya equation," Eq. (6), is more appropriate for this system. Unlike the Krichevsky-Kasarnovsky equation, it acco ‘change in the activity coefficient of the solute as a function of composition." ‘The A parameter is determined from the slope of linear plots of the left-hand side of Eq. (6) against (Yi,0.¥~1)- ‘The correlations obtained for the two parameters, Ho, and A, obtained by performing a least-squares analysis of Eq. (6), are given below. They are also illustrated in Figures 1 and 3, respectively. Hp, = 5016.29 + 31.9877T ~ 0.057691? + 3.18012 - 10°°7° @ ‘A= ~2.08184 - 10° + 2.13034 - 107 —79.81907? + 0.129917? = 1.76471 -10-°7* ®) ‘The correlation for Ho, is, as expected, nearly identical to that obtained by28 ROBERT M. ENICK AND SCOTT M. KLARA. 000 ‘cones Eon 8 000 2000 1000 ‘AICoV/G-Mole) Temperature (K) FIGURE 3. Correlation for Ain the Krichevsky-Minskaya equation. using the Krichevsky-Kasamovsky equation and by treating the partial molar volume of carbon dioxide at infinite dilution as an adjustable parameter, Eq. (5). “The pressure range associated with all three correlations neglects low-pressure data (<3.4MPa) since they are not relevant to the modeling of reservoir conditions. Slightly different values for the fitted parameters will be obtained for low-pressure data.°* EFFECT OF DISSOLVED SOLIDS ON CO, SOLUBILITY Dissolved solids in the aqueous phase are known to decrease the solubility of light gases such as CO;. Li and Nghiem® suggest that the scaled particle theory (GPT) can be used to determine the Henry's constant for these systems. Literature values®* for three parameters used in the SPT (0, a, and e) can be ‘obtained for each ion present in the brine. In order to match experimental solubility data, the o parameter of the solute is optimized. In this work, the reduction of CO, solubility due to dissolved solids was correlated to CO, solubility in pure water, as suggested by Klins.°* A data set of 167 solubilities” was obtained, for a temperature range of 298 to 523K and a presure range of 3.0 to 85.0MPa, for aqueous solutions containing sodium Chloride, calcium chloride, and unspecified brines. No trends other than total dissolved solids (TDS), such as temperature and pressure, were distinct enough to correlate from this large set of data. All ions were found to decrease solubility to a comparable extent when the TDS concentration was measured on a weight, not molar, basis. This greatly simplifies computations for compositional simula tions of CO, displacement since all ions can be simply lumped together on aCO, SOLUBILITY IN WATER AND BRINE 29 "TDS, Weight % FIGURE 4 CO, solubily in brine relative to pure H,0. ‘weight basis. Computational time requirements for reservoir simulation calcula- tions are only marginally affected by the introduction of an additional parameter, TDS, and its corresponding material balance equation. The “tracking” of brine by incorporating additional material balances for each ion used in conjunction with SPT to determine solubilities may not be a practical approach to modeling problem, even though it is more accurate. The final correlation obtained from this study, shown in Figure 4, is We0,,8 = Weoy.w* (1.0 — 4.893414 - 10-2(TDS) + 0.1302838 - 10-2(TDS)? ~ 0.187199 - 10~“(TDS)’). o CONCLUSIONS ‘The major conclusions of this study are summarized below. 1. The reference Henry's constant for the CO,/water system and the partial molar volume of CO, at infinite dilution in water have been correlated from a30 ROBERT M. ENICK AND SCOTT M. KLARA very large data base of literature data over the temperature and pressure ranges associated with miscible displacement processes. Empirical temperature. dependent expressions have been determined for (a) HZo, and A for the Krichevsky-Hinskaya equation, (b) Hgo, and DZ, for the Krichevsky- Kasarnovsky equation, and (c) H2o, for the Krichevsky-Kasarnovsky equation using the Lyckman, et al.,” correlation for Do, 2. Carbon dioxide solubilities in water are best matched in a thermodynami- cally consistent manner when the Krichevsky-Hinskaya equation is used. The temperature-dependent A parameter exhibits a wide scatter about a polynomial fit of its values at various temperatures, however. The Krichevsky-Kasarnovsky equation gives equally accurate solubilities when the partial molar volume is treated as an adjustable parameter, but the values of this parameter are inconsistent with actual values. When the correct values for the partial molar volume are used, the accuracy of the predicted CO; solubilities decreases since only one adjustable parameter, Ho,, appears in the equation. 3. An empirical correlation for the decreased solubility of CO; in an aqueous phase containing dissolved solids is presented. One hundred sixty-seven literature data points were used to develop this correlation. CO, solubility in brine relative to that in water at the same temperature and pressure is correlated with the total dissolved solids concentration. Although the correlation is easy to use in reservoir simulation since all ions are lumped together, itis characterized by a wide scatter of data and is less accurate than techniques which account for the combined effects of individual ions. NOMENCLATURE A Parameter in the Krichevsky-Iiaskaya equation, Joules/mole. fi fugacity of CO;, MPa Heo, Henry's law constant of CO;, MPa fo, reference Henry's law constant of CO;, MPa Héo, Henry's law constant of CO, at a given pressure p2, MPa M molecular weight P pressure, MPa Po Pressure where H7 is evaluated, vapor pressure of water, MPa P absolute pressure, MPa R universal gas constant, 8.314 MPa cm*/mole K T temperature, K TDS —_total dissolved solids concentration (weight percent) excluding dis- solved gases. molar volume, cm?/mole molar volume of CO; at infinite dilution, em*/moleCO; SOLUBILITY IN WATER AND BRINE 31 w solubility, weight fraction Yoo. mole fraction of CO, in the aqueous phase Subscripts 6 brine w water REFERENCES 1. Luks, K.D., Fiugibbon, P.D., and Banchero, 1-T., “Correlations of the Equilibrium Moisture Content of Air and of Mixtures of Oxygen and Nitrogen for Temperatures inthe Range of 230 0 GOK at Pressures up to 100 Atmospheres,” Ind. Eng. Chem. 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