Analyzing solubility of acid gas and light alkanes in triethylene glycol

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1 From the SelectedWorks of ali ali 208 Analyzing solubility of acid gas and light alkanes in triethylene glycol ali ali Available at:

2 Journal of Natural Gas Chemistry 17(2008)51 58 Analyzing solubility of acid gas and light alkanes in triethylene glycol Alireza Bahadori 1, Hari B. Vuthaluru 1, Saeid Mokhatab 2 1. Department of Chemical Engineering, Curtin University of Technology, GPO Box 1987, Perth, WA 6845, Australia; 2. Process Technology Manager, Tehran Raymand Consulting Engineers, Tehran, Iran [ Manuscript received June 4, 2007; revised July 20, 2007 ] Abstract: Physical solvents such as ethylene glycol (EG), diethylene glycol (DEG), and triethylene glycol (TEG) are commonly used in wet gas dehydration processes with TEG being the most popular due to ease of regeneration and low solvent losses. Unfortunately, TEG absorbs significantly more hydrocarbons and acid gases than EG or DEG. Quantifying this amount of absorption is therefore critical in order to minimize hydrocarbon losses or to optimize hydrocarbon recovery depending on the objective of the process. In this article, a new correlation that fully covers the operating ranges of TEG dehydration units is developed in order to determine the solubility of light alkanes and acid gases in TEG solvent. The influence of several parameters on hydrocarbon and acid gas solubility including temperature, pressure, and solvent content is also examined. Key words: solubility; triethylene glycol; acid gas; hydrocarbon; gas dehydration 1. Introduction Glycol dehydration of natural gas employs ethylene glycol (EG), diethylene glycol (DEG), or triethylene glycol (TEG) to remove water from the gas stream. However, the most commonly used glycol is triethylene glycol. Ethylene glycol and diethylene glycol may also be used in dehydration applications; however, EG and DEG are often not considered due to dry gas water content requirements. TEG has a higher degradation temperature and can be regenerated to a higher lean concentration with no modifications to the standard regenerator reboiler. However, EG and DEG can meet water content specifications when used with enhanced regeneration systems. Enhanced regeneration system is one that improves glycol regeneration to achieve a leaner or more concentrated glycol solution. Enhanced regeneration could be the injection of stripping gas into the reboiler, azeotropic regeneration, or other proprietary processes. The costs associated with the use of EG or DEG would be increased glycol makeup and some form of enhanced regeneration to obtain a more concentrated glycol and thus achieve the dry gas water content [1]. In previous work and in cases of multicomponent systems, study showed that equation-of-state (EOS) methods generally do a good job of determining vapor-phase properties. But accurate determination of properties for the liquid Corresponding author. Alireza.bahadori@student.curtin.edu.au phase is much more difficult, especially when the liquid contains dissimilar molecules or polar molecules such as H 2 S, CO 2, alcohols, and glycol [2]. In that article, a multicomponent system that includes polar components was evaluated, and the results showed that the Soave-Redlich-Kwong (SRK) equation of state (EOS) [3] and Non Random Two Liquids (NRTL) model [4] did not have good agreement with reported experimental data. In the other study, the numerical model was applied for vapor-solid equilibrium calculations in gas hydrate formation and the study showed that numerical approach could be an efficient method to predict vapor-solid composition and equilibrium constants [5]. In a typical dehydration plant, the regenerated glycol is pumped to the top tray of the contactor (absorber). The glycol absorbs water as it flows down through the contactor countercurrently to the gas flow. Water-rich glycol is removed from the bottom of the contactor, passes through the reflux condenser coil, flashes off most of the soluble gas in the flash tank, and flows through the rich-lean heat exchanger to the regenerator. In the regenerator, absorbed water is distilled from the glycol at near-atmospheric pressure by application of heat. The regenerated lean glycol leaving the surge drum, partially cools in the lean-rich exchanger, and pumps through the glycol cooler before being recirculated to the contactor.

3 52 Alireza Bahadori et al./ Journal of Natural Gas Chemistry Vol. 17 No Regeneration of the rich TEG solution liberates the light hydrocarbons and acid gas components. This may present an environmental or safety hazard when they are discharged from the top of the regenerator. Upon regeneration of the glycol, all absorbed gases are flashed off. From here they can be routed to fuel, flare, or gas-recovery system. Emissions from glycol dehydration units are a major environmental concern. Glycol will absorb some hydrocarbons and acid gases at the high pressure of the contactor. The amount of these compounds absorbed and consequently liberated from the glycol depends on their concentrations in the wet gas being dehydrated, the contactor s pressure and temperature. In an actual dehydration facility, the glycol is regenerated to about 99% purity or higher. The absorbed amount of gases depends on the amount of glycol circulated. If the glycol is not regenerated to this purity, then the amount of gas absorbed per unit of lean glycol circulated would be slightly less than in the proposed equations. Both temperature and pressure also affect hydrocarbon absorption. In general, the lower the temperature and the higher the pressure, the more hydrocarbons will be dissolved in the physical solvent. In some cases, however, the hydrocarbon solubility actually increases with temperature [6]. In most cases the hydrocarbon and acid gas removal is undesirable and should be minimized. More stringent emission regulations have forced the use of some methods of minimizing hydrocarbon pickup or disposal of the emissions in glycol dehydration units. Some methods for minimizing hydrocarbon absorption are: (1) decreasing the glycol circulation rate, (2) decreasing the absorber pressure, and (3) selecting a glycol that absorbs the least amount of BTEX (benzene, toluene, ethyl benzene, and xylene) or hydrocarbon if possible [7]. There are no standard sampling and analytical methods established by regulatory agencies for determining emissions from glycol dehydrators, and the methods initially used by the industry showed significant variability in results [1,8]. 2. New proposed correlation Equilibrium data and in some cases operating data are available for acid gases and hydrocarbon solubility in TEG solvent. Equation (1) presents a new correlation developed based on some experimental data reported by Jou et al. (1987) in which four coefficients are used to correlate solubility and partial pressure. The range of temperature and pressures were chosen because the conditions were similar to typical absorber conditions. Where: x = a + bp ri + cp 2 ri + dp 3 ri (1) a = A a + B a T ri + C a T 2 ri + D a T 3 ri (2) b = A b + B b T ri + C b T 2 ri + D b T 3 ri (3) c = A c + B c T ri + C c T 2 ri + D ct 3 ri (4) d = A d + B d T ri + C d T 2 ri + D dt 3 ri (5) The required data to predict tuned coefficients in Table 1 include reduced partial pressure, reduced temperature, and mole fraction of individual components in liquid phase. At first, the mole fraction of components is correlated with reduced partial pressure of components at different constant temperatures; then the calculated coefficients for these polynomials are correlated for different reduced temperatures. A practical case for gas dehydration is evaluated by this proposed approach and coefficients are tuned based on method in Reference [9]. When calculated coefficients are correlated for different temperatures by least squares method in a gas dehydration plant, the tuned coefficients are calculated, which are shown in Table 1. These coefficients are used in Equations (2) to (5). Equation (1) is a polynomial which demonstrates the variation of mole fraction vs partial pressure of individual components. The principle of the proposed correlation is based on thermodynamic properties as T r (reduced temperature) and P r (reduced pressure) for individual components, feed composition and some experimental data [6]. Then equations (6) and (7) show the mole fraction conversion of components to volumetric dimensions. Equation (6) predicts the volume of solute dissolved based on molecular weight of solute and solute mole fraction is the molecular weight of TEG and is the cubic meter of solute dissolved per kg mole of solute. Equation (7) is the volume of pure TEG and is the sp.gr. of TEG. This equation predicts the volume of pure TEG in cubic meter. V = 1 V TEG = 23645x Mx (1 x) Mx Mx (1 x) Where, V is the standard volume of acid gas or light alkane component in TEG (cubic meter), M is the molecular weight of acid gas or light alkane components, and V TEG is the volume of TEG (cubic meter). Equation (8) calculates the rate of liberated gas per rate of TEG circulation. Considering equations (6) and (7), liberated gas flowrate can be calculated as: Q = (6) (7) V V TEG (q TEG ) (8)

4 Journal of Natural Gas Chemistry Vol. 17 No Where, q TEG is circulated TEG (cubic meter per day) and Q is the rate of liberated gas. In the above equations, x is the mole fraction of acid gas or light alkane component in TEG, P r and T r are reduced partial pressure and reduced temperature of each component (i), respectively. Tuned coefficients in equations (2) to (4) are also given in Table 1. These tuned coefficients are changed if more accurate experimental data are available. Table 1. Tuned coefficients in Equations (2) to (5) Coefficient Different solutes H 2 S CO 2 CH 4 C 2 H 6 C 3 H 8 A a B a C a D a A b B b C b D b A c B c C c D c A d B d C d D d The pressure and temperature limitations of the model applicability are up to kpa and up to 130 C for CH 4, respectively. Concerning C 2 H 6, the partial pressure limits of applicability are up to 7000 kpa and temperature is limited to 100 C. For C 3 H 8 component, the partial pressure range is up to 1000 kpa and temperature is limited to 80 C. For H 2 S, the partial pressure range is up to kpa and temperature is limited to 100 C. For CO 2, the partial pressure range is up to kpa and temperature is limited to 100 C. 3. Case study Table 2 shows the composition and operating condition of a typical contactor feed. In this case study the solubility of acid-gas in TEG in different TEG circulation rates and different contactor temperatures and pressures are evaluated and the effect of TEG circulation rate on solubility of acid gases and light alkane components are analyzed by proposed correlation and some improvements in previously developed equations are finally presented. 4. Results Figure 1 shows the new correlation results for acid-gas absorbed in TEG versus contactor total pressure at different TEG circulation flow rates. It also shows the trend of solubility of acid gases in TEG for different TEG circulation rates Table 2. Typical composition for wet gas inlet to contactor Component mol % C C C IC NC IC NC NC H 2 O H 2 S CO N C C 7+ molecular weight C 7+ specific gravity P (kpa) 3700 T ( C) 42 Mass flow rate for inlet water content (kg h 1 ) and contactor pressures. The rate of liberated acid gases increases by increasing TEG circulation rate and contactor pressure and decreasing the contactor temperature. Figure 2 shows the new correlation results for light alkanes including CH 4,C 2 H 6,andC 3 H 8 absorbed in TEG versus

5 54 Alireza Bahadori et al./ Journal of Natural Gas Chemistry Vol. 17 No Figure 1. New correlation results for acid-gas absorbed in TEG vs contactor pressure at different TEG circulation rates total contactor pressure at different TEG circulation rates. It also shows the trend of solubility of light hydrocarbons in TEG for different TEG circulation rates and contactor pressures. The rate of liberated light hydrocarbon gases increases by increasing TEG circulation rate and contactor pressure and decreasing the contactor temperature. Figure 2. New correlation results for light hydrocarbons absorbed in TEG vs contactor pressure and at different TEG circulation rates Tables 3 and 4 present comparisons between some experimental data for H 2 S and CO 2 solubility in TEG with the obtained results of the new developed model. As can be seen, the average absolute deviation percentage of the new model for predicting H 2 SandCO 2 solubility in TEG are % and %, respectively. Table 3. Comparing new model results for predicting the solubility of H 2 S in TEG with experimental data [6] Pressure Temperature H 2 S mole fraction H 2 S mole fraction Absolute deviation Average of absolute deviation (%) %AADP = 100% NOP NOP i ( ) Calculated value Experimental value 1 = %, in which AADP= Average absolute deviation percent, NOP= number of points i

6 Journal of Natural Gas Chemistry Vol. 17 No Table 4. Comparing new model results for predicting the solubility of CO 2 in TEG with experimental data [6] Pressure Temperature CO 2 mole fraction CO 2 mole fraction Absolute deviation Average of absolute deviation (%) Tables 5 to 7 also give comparisons between some experimental data for methane, ethane, and propane solubilities in TEG with the obtained results of the new developed model. As can be seen, the average absolute deviation percentage of the new model for predicting methane, ethane, and propane solubilities in TEG are %, 3.139%, and %, respectively. In the light of the above and considering the simplicity of the proposed correlation, it is recommended to use the new developed model instead of using routine graphical methods or conventional commercial softwares. Note that since dehydrators usually operate at temperatures of less than 60 C, there was no practical need to include temperatures higher than 75 C in the graphs of this work. As can be seen from the above-mentioned figures, the solubility of acid gases in TEG is more than light alkane solubility, however, since the mole fraction of light alkane in contactor s feed gas is more than acid gas, the solubility of light

7 56 Alireza Bahadori et al./ Journal of Natural Gas Chemistry Vol. 17 No alkane is therefore important and has to be accurately considered in design of TEG dehydration units. The new developed correlation has been demonstrated to match the experimental solubility data very closely, where it will be used to investigate factors affecting hydrocarbon and acid gas solubility in TEG. Table 5. Comparing new model results for predicting the solubility of CH 4 in TEG with experimental data [6] Pressure Temperature CH 4 mole fraction CH 4 mole fraction Absolute deviation Average of absolute deviation (%)

8 Journal of Natural Gas Chemistry Vol. 17 No Table 6. Comparing new model results for predicting the solubility of C 2 H 6 in TEG with experimental data [6] Pressure Temperature C 2 H 6 mole fraction C 2 H 6 mole fraction Absolute deviation Average of absolute deviation (%) Table 7. Comparing new model results for predicting the solubility of C 3 H 8 in TEG with experimental data [6] Pressure Temperature C 3 H 8 mole fraction C 3 H 8 mole fraction Absolute deviation E E E Average of absolute deviation (%)

9 58 Alireza Bahadori et al./ Journal of Natural Gas Chemistry Vol. 17 No Conclusions In this article, a new correlation that fully covers the operating ranges of TEG dehydration units is developed in order to determine the solubility of light alkanes and acid gases in TEG solvent. The influence of several parameters on hydrocarbon and acid gas solubility including temperature, pressure, and solvent content is also examined. The new developed correlation has been demonstrated to match the experimental solubility data very closely, where it will be used to investigate factors affecting hydrocarbon and acid gas solubility in TEG. In the light of the above and considering the simplicity of the proposed correlation, it is recommended to use the new developed correlation instead of using routine graphical methods or conventional commercial softwares. Acknowledgements The lead author acknowledges the Australian Department of Education, Science and Training for Endeavour International Postgraduate Research Scholarship and Office of Research & Development at the Curtin University of Technology, Perth, Western Australia for providing Curtin University Postgraduate Scholarship. Nomenclature A temperature coefficient B temperature coefficient C temperature coefficient D temperature coefficient x solute mole fraction T r reduced temperature P r reduced partial pressure V standard volume of acid gas or light alkane component in TEG (cubic meter) M molecular weight of acid gas or light alkane components V TEG volume of TEG (cubic meter) q TEG circulated TEG (cubic meter per day) Q total liberated gas (cubic meter) i solute component index References [1] Grizzle P L. Paper presented at the SPE/EPA Exploration & Production Environmental Conference, San Antonio, T X, USA (March 7-10, 1993) [2] Bahadori A. Chemical Engineering, 2007, 114(8): 47 [3] Soave G. Chem Eng Sci, 1972, 27(6): 1197 [4] Renon H, Prausnitz J M. AIChEJ, 1968, 14(1): 135 [5] Bahadori A. J Natur Gas Chem, 2007, 16(1): 16 [6] Jou F Y, Deshmukh R D, Otto F D, Mather A E. Fluid Phase Equilibria, 1987, 36: 121 [7] Ebeling H O, Lyddon L G, Covington K K. Paper presented at the 77 th GPA Annual Convention, Gas Processors Association, Tulsa, OK, USA (1998) [8] JouFY,OttoFD,MatherAE.The Canadian Journal of Chemical Engineering, 1994, 72(1): 130 [9] Bahadori A, Mokhatab S, Towler B F. J Natur Gas Chem, 2007, 16(4): 349

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