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Rate-Based Model of the CO2 Capture Process by DEA using Aspen Plus
Copyright (c) 2008 by Aspen Technology, Inc. All rights reserved. Aspen Plus, the aspen leaf logo and Plantelligence and Enterprise Optimization are trademarks or registered trademarks of Aspen Technology, Inc., Cambridge, MA. All other brand and product names are trademarks or registered trademarks of their respective companies. This document is intended as a guide to using AspenTech's software. This documentation contains AspenTech proprietary and confidential information and may not be disclosed, used, or copied without the prior consent of AspenTech or as set forth in the applicable license agreement. Users are solely responsible for the proper use of the software and the application of the results obtained. Although AspenTech has tested the software and reviewed the documentation, the sole warranty for the software may be found in the applicable license agreement between AspenTech and the user. ASPENTECH MAKES NO WARRANTY OR REPRESENTATION, EITHER EXPRESSED OR IMPLIED, WITH RESPECT TO THIS DOCUMENTATION, ITS QUALITY, PERFORMANCE, MERCHANTABILITY, OR FITNESS FOR A PARTICULAR PURPOSE. Aspen Technology, Inc. Ten Canal Park Cambridge, MA 02141-2201 USA Phone: (1) (617) 949-1000 Toll Free: (1) (888) 996-7001 Fax: (1) (617) 949-1030 URL: http://www.aspentech.com
0 Description First version Revision History 3 .Revision History Version V7.
........................................5 1 Components .................16 6 Simulation Results .....................................................................................................................6 2 Process Description................................................23 4 Contents ..........................................................................20 7 Conclusions .............................7 3 Physical Properties................................................................................................................................................................................................................................................................................................................................................................................................................13 5 Simulation Approaches.......................................22 References ...................................................8 4 Reactions ...........................................Contents Introduction ............................................
CO2 and H2S. The operation data from a natural gas treating unit at Pyote. C2H6.Introduction This document describes an Aspen Plus rate-based model of the CO2 capture process by DEA (Diethanolamine) from a gas mixture of CH4. C3H8. Transport property models and model parameters have been validated against experimental data from open literature. Thermophysical property models and reaction kinetic models are based on the works of Aspen Technology(2007) and Rinker(1996). N2. Texas(1975) were used to specify feed conditions and unit operation block specifications. The model presented here includes the following key features: • • • • • True species including ions Electrolyte NRTL method for liquid and RK equation of state for vapor Concentration-based reaction kinetics Electrolyte transport property models Rate-based models for absorber and stripper with valve trays Introduction 5 . The model consists of an absorber and a stripper.
1 Components The following components represent the chemical species present in the process: Table 1. Components Used in the Model ID H2O DEA CO2 H3O+ OHHCO3CO3-2 DEAH+ DEACOOH2S HSS-2 CH4 C2H6 C3H8 N2 Type Conventional Conventional Conventional Conventional Conventional Conventional Conventional Conventional Conventional Conventional Conventional Conventional Conventional Conventional Conventional Conventional Name WATER DIETHANOLAMINE CARBON-DIOXIDE H3O+ OHHCO3CO3-DEA+ DEACOOHYDROGEN-SULFIDE HSS-METHANE ETHANE PROPANE NITROGEN Formula H2O C4H11NO2-1 CO2 H3O+ OHHCO3CO3-2 C4H12NO2+ C5H10NO4H2S HSS-2 CH4 C2H6 C3H8 N2 6 1 Components .
However. Data of the Pyote Unit Absorber Diameter Tray Stripper Diameter Tray Feeds and Products Sour Gas to Absorber Lean Amine to Absorber Rich Amine to Stripper CO2 in Sour Gas H2S in Sour Gas CO2 in Sweet Gas H2S in Sweet Gas DEA solution 2.013(mole fraction) 0.69%(wt) 72 inch 31 66 inch 20 2 Process Description 7 .00054(mole fraction) 150 ppm (mole fraction) 0.15 ppm (mole fraction) 28. only one absorber and one stripper data are reported.2 Process Description The Pyote Unit flowsheet for CO2 capture by DEA includes three absorbers and two strippers.92 MM scfh 188 gpm 380 gpm 0. Table 2 represents the typical operation data: Table 2.
The NRTL parameters were regressed against VLE data from Maddox(1987. The interaction parameter VLQKIJ for the quadratic mixing rule between DEA and H2O is regressed against experimental density data of the DEAH2O system from Maham(1994). the activity coefficient basis for the Henry’s components is chosen to be Aqueous. Therefore. CO2 and H2S are treated as Henry-components (solutes) to which Henry’s law is applied. The three option codes for MUL2JONS are set to: 1 (mixture viscosity weighted by mass fraction). instead of in mixed solvents. The Clarke model parameter VLCLK/1 is also regressed for main electrolytes (DEAH+. The interaction parameters between DEA and H2O in the ASPEN liquid mixture viscosity model. Hsu(1997). 1989)[4. Specifications of these models include: • For liquid molar volume. • For liquid viscosity.3 Physical Properties The Electrolyte NRTL method and RK equation of state are used to compute liquid and vapor properties respectively in this rate-based DEA model. is used with the mass fraction based ASPEN liquid mixture viscosity model for the solvents. C2H6. 5] for CO2 with DEA. 1 (always use Jones and Dole equation when the parameters are available). CH4. In the reactions calculations. C3H8. CO 3 ) against experimental density data of the DEA-H2O-CO2 system from Weiland(1998). in calculating the unsymmetric activity coefficients (GAMUS) of the solutes. 1989)[4. Weiland(1998). and Mandal(2003). HCO 3 ). are regressed against experimental DEA-H2O viscosity data from Oyevaar(1989). Henry’s constants are retrieved from Aspen Plus databanks for these components with water and are regressed against CO2 solubility data from Maddox(1987.are regressed − − −2 8 3 Physical Properties .5]. and 2 (ASPEN liquid mixture viscosity model). the Jones-Dole electrolyte correction model. is used with option code of 1 to use the quadratic mixing rule for solvents. the infinite dilution activity coefficients will be calculated based on infinite-dilution condition in pure water. the Clarke model. MUKIJ and MULIJ. (DEAH+. The Jones-Dole model parameters. called MUL2JONS in Aspen Plus. IONMUB. DEACOO ) and (DEAH+. respectively. N2. for DEAH+ and DEACOO. Rinker(1994). called VAQCLK in Aspen Plus. The liquid molar volume and transport property models have been updated and their model parameters regressed from literature experimental data.
the Riedel electrolyte correction model. the aqueous phase heat of formation at infinite dilution and 25°C (DHAQFM) for DEAH+ and DEACOOand the heat capacity at infinite dilution (CPAQ0) for DEAH+ and DEACOO. For thermal conductivity. The estimation results of various transport and thermophysical properties are summarized in Figures 1-7: 1200 1150 EXP DEA EXP DEA EXP DEA EXP DEA EST DEA EST DEA EST DEA EST DEA 10w t% 20w t% 30w t% 40w t% 10w t% 20w t% 30w t% 40w t% 1100 Density. respectively. is used.1 0. is used with option code of 1 (mixture viscosity weighted by mass fraction). experimental data from Weiland (1998) 3 Physical Properties 9 . called DL0NST in Aspen Plus. that of CO 3 is regressed against K2CO3-H2O viscosity data from Pac et al. • For liquid surface tension.are adjusted to fit to the literature data on heat of solution from Carson(2000) and heat capacity from Weiland(1997).2 0.3 0.against DEA-H2O-CO2 viscosity data from Weiland(1998). called SIG2ONSG in Aspen Plus. called KL2RDL in Aspen Plus. and that of HCO3.(1984). kg/m3 1050 1000 950 900 0 0. Liquid Density of DEA-CO2-H2O at 298. m ol/m ol Figure 1. the Onsager-Samaras model. −2 • • In addition to the updates to the above properties. the Nernst-Hartley model. For binary diffusivity.5 CO2 Loading.15K. is used with its option codes being -9 (exponent in mixing rule) and 1 (electrolyte system). No additional adjusted parameters are used in the surface tension model and the estimation results are somewhat higher than the experimental data from Weiland(1996) (Figure 3).is regressed against KHCO3-H2O viscosity data from Palaty(1992).4 0.
1 0 0.3 0. mPaS 1 EXP DEA EXP DEA EXP DEA EST DEA EST DEA EST DEA 0. Liquid Viscosity of DEA-CO2-H2O at 298. m ol/m ol Figure 3.10 Viscosity.30 0.15K.1 0.00 EXP DEA EST DEA EXP DEA EST DEA EXP DEA EST DEA EXP DEA EST DEA 0.20 0. Surface tension of DEA-CO2-H2O at 298. mN/m 70 60 50 40 30 20 10 0 0. experimental data from Weiland (1998) 100 90 80 Surface Tension. m ol/m ol Figure 2. experimental data from Weiland (1996) 10 3 Physical Properties .15K.10 10w t% 10w t% 20w t% 20w t% 30w t% 30w t% 40w t% 40w t% 0.4 0.2 20w t% 30w t% 40w t% 20w t% 30w t% 40w t% 0.5 CO2 Loading.50 CO2 Loading.40 0.
5 0. experimental data from Weiland (1997) 3 Physical Properties 11 .2 0.3 0.6 Thermal Conductivity. Liquid Heat Capacity of DEA-CO2-H2O at 298.1 10w t% 20w t% 30w t% 40w t% 0. Liquid Thermal Conductivity of DEA-CO2-H2O at 298.4 0.15K. Watt/m-K 0.15K Figure 5. mol/mol Figure 4.0.3 0.1 0 CO2 Loading.4 0.5 0.6 0.2 DEA DEA DEA DEA 0 0.
experimental data from Carson (2000) Figure 7. Heat of Solution of DEA-CO2-H2O at 298.Figure 6.20).15K. CO2 partial pressure of DEA-CO2-H2O (DEA mass fraction = 0. experimental data from Maddox (1989) 12 3 Physical Properties .
In addition.and CO2 with DEA. a REACTION model named DEA-REA has been created. It can associate with H3O+ to form DEAH+ ion and can also react with CO2 to form carbamate ion DEACOO-. which is used in calculations of the absorber and stripper by specifying it in the Reaction part of the absorber and stripper specifications. Chemistry ID: DEA 1 2 3 4 5 6 7 Equilibrium Equilibrium Equilibrium Equilibrium Equilibrium Equilibrium Equilibrium DEAH + + H 2 O ↔ DEA + H 3 O + − CO 2 + 2H 2 O ↔ H 3 O + + HCO 3 − − HCO 3 + H 2 O ↔ H 3 O + + CO 3 2 − DEACOO − + H 2 O ↔ DEA + HCO 3 2H 2 O ↔ H 3 O + + OH − H 2 O + H 2 S ↔ HS − + H 3 O + H 2 O + HS − ↔ S −2 + H 3 O + 4 Reactions 13 . Chemical equilibrium is assumed with all the ionic reactions in the CHEMISTRY DEA. A. In DEA-REA. as shown in Figure 8. DEA Molecular Structure The electrolyte solution chemistry has been represented with a CHEMISTRY model with ID of DEA. which is used as a global electrolyte calculation option in the simulation by specifying it on the Global sheet of the Properties | Specifications form. Figure 8.4 Reactions DEA is a secondary ethanolamine. all reactions are assumed to be in chemical equilibrium except those of CO2 with OH.
(1) ai = The stoichiometric number of component i in the reaction equation. Reaction ID: DEA-REA 1 2 3 4 5 6 7 8 9 Equilibrium Equilibrium Equilibrium Kinetic Kinetic Kinetic Kinetic DEAH + + H 2 O ↔ DEA + H 3 O + 2H 2 O ↔ H 3 O + + OH − − − HCO 3 + H 2 O ↔ H 3 O + + CO 3 2 − CO 2 + OH − → HCO 3 − HCO 3 → CO 2 + OH − DEA + CO 2 + H 2 O → DEACOO .13]. the concentration basis is Molarity and the factor n is zero.B.(1988) and Jou et al. the reduced power law expression is used: r = kT n exp ( − E N ai )∏ C i RT i =1 (2) In this work. the power law expressions are used for the rate-controlled reactions (reactions 47 in DEA-REA) and the general power law expression is: ⎡⎛ − E ⎞⎛ 1 1 ⎞⎤ N ai n r = k (T To ) exp ⎢⎜ ⎟⎜ − ⎟⎥∏ C i ⎟ ⎝ R ⎠⎜ T To ⎠⎦ i =1 ⎝ ⎣ Where: r = Rate of reaction. In addition. R = Gas low constant.(1982. In equation (2). 1993)[11. The kinetic parameters for reactions 4-7 in Table 3 are derived from the work of Rinker(1996). If To is not specified. E = Activation energy. n = Temperature exponent. The DEA concentration range of the data of 14 4 Reactions . k = Pre-exponential factor. T0 = Reference temperature. Ci = Concentration of component i. N = Number of components in the reaction. k and E are given in Table 3.+ H 3 O + → DEA + H 2 O + CO 2 H 2 O + H 2 S ↔ HS − + H 3 O + H 2 O + HS − ↔ S −2 + H 3 O + Equilibrium Equilibrium The equilibrium expressions for the reactions are taken from the work of Austgen et al. the reduced expressions are used.+ H 3 O + DEACOO .12. T = Absolute temperature.
(1956) The kinetic parameters for reaction 5 are calculated by using the kinetic parameters of reaction 4 and the equilibrium constants of the reversible reactions 4 and 5.Rinker is 0. The kinetic parameters for reaction 4 are taken from the work of Pinsent et al. Parameters k and E in Equation (2) Reaction No. Table 3.25-2. 4 5 6 7 k 4.34e+17 E (cal/mol) 13249 29451 5072 11497 4 Reactions 15 .8 M and the temperature range is 292-343 K.32e+13 2.38e+17 6480000 1. these conditions are the operating conditions of the absorber modeled in this work.
Simulation Flowsheet – The Pyote Unit has been modeled with the following simulation flowsheet in Aspen Plus as shown in Figure 9.5 Simulation Approaches The natural gas treating unit at Pyote is simulated in this work and is described in this section. Rate-Based DEA Simulation Flowsheet in Aspen Plus 16 5 Simulation Approaches . GASOU T CO2OU T LEANIN ABSORBER GASIN RICHOUT LEANOUT RICHIN STRIPPER Figure 9.
001 m3. Reaction: Reaction ID is DEA-REA for all stages. Weir height: 0.001. Table 4.1 and 0. These estimates are intended to aid convergence 5 Simulation Approaches 17 . Aspen Plus Unit Operation Blocks Used in the Rate-Based MEA Model Unit Operation Absorber Aspen Plus Block RadFrac Comments / Specifications 1. Heat transfer coefficient method: Chilton and Colburn 12. Film resistance: Discrxn for liquid film. (1983) 13. Top Pressure: 900 psig 4. Additional discretization points for liquid film: 0. 20 Stages 3. Interfacial area method: Scheffe and Weiland (1987) 10. Holdup=0. which is intended to aid convergence 5. Tray Type: Glitsch Ballast 6. Holdup is used. Holdup scale factor: 1 14.Unit Operations – The major unit operation models have been represented by Aspen Plus Blocks as outlined in Table 4. Interfacial area factor: 0. Flow model: Mixed 17. Calculation type: Rate-Based 2. Estimates: provide temperature estimates for all stages.72 11. 0. Film for vapor film 15.01. 0. Mass transfer coefficient method: Scheffe and Weiland (1987) 9. and in this file. when calculation type is equilibrium. Tray Diameter: 66 inch 7.06 m 8. Holdup correlation: Bennett et al.5 16. 0.0001.
Film resistance: Discxrn for liquid film.03kmol/s with final value of 0. when calculation type is equilibrium. Estimates: provide temperature estimates for all stages. which is intended to aid convergence. Top Pressure: 9. 33 Stages 3. Partial vapor condenser 4. Reaction: Reaction ID is DEA-REA for all stages.5 20.5K 10. Holdup=0. Tray Diameter: 72 inch 13. and in this file. Design specs: Stage 1 temperature = 291.001 m3. Tray Type: Glitsch Ballast 12. Flow model: Mixed 21. Vary: Distillate rate 11. Calculation type: Rate-Based 2. Mass transfer coefficient method: Scheffe and Weiland (1987) 14. 0. Mole reflux rates: 0. 0. 0. (1983) 18.04kmol/sec 7.02804509kmol/s obtained by Design-Spec 1 6.0001.Unit Operation Stripper Aspen Plus Block RadFrac Comments / Specifications 1. Additional discretization points for liquid film: 0. Heat transfer coefficient method: Chilton and Colburn 17.01.1 and 0. Film for vapor film 19. Interfacial area factor: 1 16. Interfacial area method: Scheffe and Weiland (1987) 15. Mole distillate rate: initialized at 0.8 psig 8. 9. Kettle reboiler 5. these estimates are intended to aid convergence 18 5 Simulation Approaches .001. Holdup is used. Holdup correlation: Bennett et al.
7118 0.063 0.0001 0 0 0 0 212 10 380 gal/min Mole-Frac 0.01 102 900 188 gal/min Mass-Frac 0. Feed streams conditions are summarized in Table 5. CO2 and H2S and liquid solvent stream LEANIN containing aqueous DEA solution with few CO2 loaded in.924 0.016 0.026 0.91 0.2869 0. N2.Feeds to the absorber are gas stream GASIN containing CH4. Feed to the stripper is rich solvent stream RICHIN containing aqueous DEA solution with absorbed CO2.Streams . Feed specifications Stream ID Substream: MIXED Temperature: F Pressure: psig Total flow H2O DEA CO2 H2S CH4 C2H6 C3H8 N2 72 900 3689 kmol/hr Mole-Frac 0 0 0.013 0.001 0 0 0 0 GASIN LEANIN RICHIN 5 Simulation Approaches 19 .00054 0. Table 5.0012 0. C2H6. C3H8.036 0.
01 0.42 Measurement Rate-Based DEA Model 20 6 Simulation Results . The measured versus calculated absorber and stripper liquid temperature profiles are presented in Figures 10 and 11. Key simulation results are presented in Table 6. steam/ gal. lbs. MolAcidGas/MolDEA Reboiler duty.85 0.0. respectively. solution 0.87 150 ppm 0.6 Simulation Results The simulation was performed using Aspen Plus V7.50 178ppm 0. MolAcidGas/MolDEA Stripper Loading of LEANOUT.007 0. circ. Table 6. Key Simulation Results Variable Absorber CO2 mole fraction in GASOUT Loading of RICHOUT.
The Stripper Liquid Temperature Profile 6 Simulation Results 21 . The Absorber Liquid Temperature Profile 250 200 Temperature. F 100 Measure 50 AspenPlus: Liquid AspenPlus: Vapor 0 0 5 10 Stage num ber 15 20 Figure 10. F 150 Measurement 100 AspenPlus: Liquid AspenPlus: Vapor 50 0 5 10 15 20 25 30 35 Stage number Figure 11.200 150 Temperature.
plant and equipment design. 22 7 Conclusions . The model is meant to be used as a guide for modeling the CO2 capture process with DEA. You may use it as a starting point for more sophisticated models for process development. debottlenecking. rate-based multi-stage simulation with Aspen Rate-Based Distillation which incorporates heat and mass transfer correlations accounting for columns specifics and hydraulics. Key features of this rigorous simulation include electrolyte thermodynamics and solution chemistry. rigorous transport property modeling. among others.7 Conclusions The rate-based DEA model provides a rate-based rigorous simulation of the process. reaction kinetics for the liquid phase reactions.
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