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1 Ionic Liquid Design and Process Simulation for Decarbonization of Shale Gas XinyanLiu,, Ying Huang, Yongsheng Zhao, RafiqulGani, XiangpingZhang, *, SuojiangZhang *, Beijing Key Laboratory of Ionic Liquids Clean Process, State Key Laboratory of Multiphase Complex Systems, Key Laboratory of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing , China Sino-Danish Center for Education and Research, University of Chinese Academy of Sciences, Beijing , China Department of Chemical & Biochemical Engineering, Technical University of Denmark, DK 2800 Kgs. Lyngby, Denmark Supplementary material 1
2 Supporting Information Table S1... Page 2 Table S2... Page 2 Table S Page 3 Table S4... Page 3 Table S5... Page 3 Table S6... Page 4 Table S7... Page 4 Figure S1.. Page 5 Table S8... Page 5-10 Figure S2.. Page 11 Table S9... Page Figure S3.. Page 15 Table S10. Page Figure S4.. Page 19 Table S11. Page 20 Table S12. Page 21 Table S13. Page 22 Table S14. Page 23 1
3 Table S1 CO 2 henry s constant in 90 kinds of ionic liquids T=303.15K [HOemim] [Emim] [Bmim] [Hmim] [Omim] [MeButPyrr] [N4111] [N-bupy] [Hmpy] [FEP] [TCA] [Tf 2 N] [DCA] [DEP] [C 2 SO 4 ] [OTF] [CH 3 SO 4 ] [NO 3 ] [BF 4 ] Table S2 CH 4 henry s constant in 90 kinds of ionic liquids T=303.15K [HOemim] [Emim] [Bmim] [Hmim] [Omim] [MeButPyrr] [N4111] [N-bupy] [Hmpy] [FEP] [DEP] [Tf 2 N] [C 2 SO 4 ] [CH 3 SO 4 ] [OTF] [NO 3 ] [TCA] [DCA] [BF 4 ]
4 Table S3 Scalar property parameters of [bmim][ntf 2 ] IL Parameter Units Data Standard boiling point K Critical temperature K Critical pressure bar 21.7 Critical volume cm 3 /mol Acentric factor / Table S4 Henry s constant parameters in binary system Parameters CO 2 CH 4 C C C C Table S5 Comparison of predicted value and experimental value for CO 2 Temperature (K) Solubility x Predicted P (bar) Calculated P (bar) AARD 8.54% 3
5 Table S6 Comparison of predicted value and experimental value for CH 4 Temperature (K) Solubility x Predicted P (bar) Calculated P (bar) AARD 4.35% Table S7 Energy and solvent consumption of different components of raw gas VCO 2 :VCH 4 20%:80% 40%:60% 60%:40% 80%:20% IL kg/h Lean load mol CO 2 /mol IL C1/kW P1/kW Electricity (kwe) Heat duty (kwth) Flash TEC/kW SEC/MJ/kgCH SEC/MJ/kgCO
6 Figure S1 Typical Decarbonization Process Flow Sheet using MDEA Table S8(a) Operation parameters of key equipment in MDEA processes Items Unit Value Absorber Pressure of the column bottom bar 60 Gas inlet temperature o C 20 Gas outlet temperature o C 24.5 Stage number 7 Flash (F101) Pressure bar 14 Temperature o C 25 Regenerator Stage number 10 Reflux ratio 1.3 Pressure bar 1 Top temperature o C Bottom temperature o C 59.5 Heat exchanger (E) Hot stream inlet temperature o C Hot stream outlet temperature o C 65 Cold stream inlet temperature o C 55 Cold stream outlet temperature o C 82.7 Heat exchanger (E101) Inlet temperature o C 65 Outlet temperature o C 40 Purified shale gas CH 4 mole fraction CO 2 mole fraction
7 Table S8(b) Temperature, Pressure and Vapor and Liquid Flow Rate Profiles of the Absorber of the Modified MDEA Process Stage Temperature Pressure Liquid from (Mole) Vapor from (Mole) C bar kmol/hr kmol/hr Table S8(c) Vapor and Liquid Composition Profiles of the Absorber of the MDEA Process Vapor (mole fraction) Stage MDEA H 2 O CO 2 CH 4 N 2 C 2 H 6 C 3 H 8 C 4 H C 5 H E E E E E E E
8 Liquid (mole fraction) Stage MDEA H 2O CO 2 H 3O + OH - HCO 3 - CO 3-2 MDEAH + CH 4 N 2 C 2H 6 C 3H 8 C 4H C 5H E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E-07 7
9 Table S8(d) Temperature, Pressure and Vapor and Liquid Flow Rate Profiles of the Regenerator of the Modified MDEA Process Stage Temperature Pressure Heat duty Liquid from Vapor from (Mole) (Mole) C bar Watt kmol/hr kmol/hr Table S8(e) Vapor and Liquid Composition Profiles of the Regenerator of the MDEA Process Vapor (mole fraction) Stage MDEA H 2O CO 2 CH 4 N 2 C 2H 6 C 3H 8 C 4H C 5H E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E-19 8
10 Liquid (mole fraction) Stage MDEA H 2O CO 2 H 3O + OH - HCO 3 - CO 3-2 MDEAH + CH 4 N 2 C 2H 6 C 3H 8 C 4H C 5H E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E-24 9
11 Table S8(f) Stream results of the flowsheet for MDEA Decarbonization ACIDGAS GASIN GASOUT LEANIN RICHOUT Temperature o C Pressure bar Vapor Frac Mass Flow kg/hr Volume Flow cum/hr Enthalpy Gcal/hr Density kg/cum Mass Flow MDEA kg/hr H 2 O kg/hr CO 2 kg/hr H 3 O + kg/hr OH- kg/hr HCO 3- kg/hr CO -2 3 kg/hr MDEAH + kg/hr CH 4 kg/hr N 2 kg/hr C 2 H 6 kg/hr C 3 H 8 kg/hr C 4 H kg/hr C 5 H kg/hr
12 Figure S2 IL-based Decarbonization Flow Sheet (two single-stage) Table S9(a) Operation parameters of key equipment in IL-based decarbonization process (two single-stage) Items Unit Value Absorber Pressure of the column bottom bar 60 Gas inlet temperature o C 20 Gas outlet temperature o C 24.5 Stage number 10 Flash-1 Pressure bar 15 Temperature o C 25 Flash-2 Pressure bar 1 Temperature o C 27 Heat exchanger (E) Inlet temperature o C 27 Outlet temperature o C 20 Purified shale gas CH 4 mole fraction CO 2 mole fraction
13 Table S9(b) Temperature, Pressure and Vapor and Liquid Flow Rate Profiles of the Absorber of the IL-based Decarbonization Process (two single-stage) Stage Temperature Pressure Liquid from (Mole) Vapor from (Mole) C bar kmol/hr kmol/hr Table S9(c) Vapor and Liquid Composition Profiles of the Absorber of the IL-based Decarbonization Process (two single-stage) Vapor (mole fraction) Stage CO2 BMIMTF2N CH4 C2H6 C3H8 N2 H2O C4H10 C5H E E E E E E E E E E E E E E E E E E E E
14 Liquid (mole fraction) Stage CO2 BMIMTF2N CH4 C2H6 C3H8 N2 H2O C4H10 C5H E E E E E E E E E E E E E E E E E E E E
15 Table S9(d) Stream results of the flowsheet for IL-based Decarbonization (two single-stage) ACIDGAS Bmim Tf 2 N GASIN GASOUT RICHOUT Temperature o C Pressure bar Vapor Frac Mole Flow kmol/hr Mass Flow kg/hr Volume Flow cum/hr Enthalpy Gcal/hr Mass Flow kg/hr CO BmimTf 2 N CH C 2 H C 3 H N H 2 O C 4 H C 5 H
16 Figure S3 IL-based decarbonization flow sheet (Multi-stage flash) Table S10(a) Operation parameters of key equipment in IL-based decarbonization process (Multi-stage flash) Items Unit Value Absorber Pressure of the column bottom bar 60 Gas inlet temperature o C 20 Gas outlet temperature o C 23.6 Stage number 10 Flash-1 Pressure bar 55 Temperature o C 25 Flash-2 Pressure bar 40 Temperature o C 25 Flash-3 Pressure bar 30 Temperature o C 25 Flash-4 Pressure bar 0.4 Temperature o C 25 Heat exchanger (E-1) Inlet temperature o C 25 Outlet temperature o C 20 Purified shale gas CH 4 mole fraction CO 2 mole fraction
17 Table S10(b) Temperature, Pressure and Vapor and Liquid Flow Rate Profiles of the Absorber of the IL-based decarbonization Process (Multi-stage flash) Stage Temperature Pressure Liquid from (Mole) Vapor from (Mole) C bar kmol/hr kmol/hr Table S10(c) Vapor and Liquid Composition Profiles of the Absorber of the IL-based Decarbonization Process (Multi-stage flash) Vapor (mole fraction) Stage CO2 BMIMTF2N CH4 C2H6 C3H8 N2 H2O C4H10 C5H E E E E E E E E E E E E E E E E E E E E
18 Liquid (mole fraction) Stage CO2 BMIMTF2N CH4 C2H6 C3H8 N2 H2O C4H10 C5H E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E E-06 17
19 Table S10(d) Stream results of the flowsheet for IL-based Decarbonization (Multi-stage flash) ACIDGAS BMIMTf2N GASIN GASOUT RICHOUT Temperature C Pressure bar Vapor Frac Mole Flow scmh Mass Flow kg/hr Volume Flow cum/sec Enthalpy Gcal/hr Mass Flow kg/hr CO BMIMTF2N CH C2H C3H N H2O C4H C5H
20 Figure S4 Flowsheet of different raw gas component for IL-based Decarbonization (two single-stage) 19
21 Table S11 Stream results of the flowsheet for IL-based Decarbonization (two single-stage) (raw gas V CO2 :V CH4 =20%:80%) ACIDGAS BMIMNTF2 GASIN GASOUT LEAN RICHOUT Temperature C Pressure bar Vapor Frac Mole Flow kmol/hr Mass Flow kg/hr Volume Flow cum/hr Enthalpy Gcal/hr Mass Flow kg/hr CO BMIMTF 2 N trace trace trace trace trace trace CH Mass Frac CO BMIMTF 2 N trace trace trace trace trace trace CH PPM PPM PPM PPM Mole Flow kmol/hr CO BMIMTF 2 N trace trace trace trace trace trace CH Mole Frac CO BMIMTF 2 N trace trace 0.82 trace trace trace trace CH PPM PPM PPM
22 Table S12 Stream results of the flowsheet for IL Decarbonization (two single-stage) (raw gas V CO2 :V CH4 =40%:60%) ACIDGAS BMIMNTF2 GASIN GASOUT LEANOUT RICHOUT Temperature C Pressure bar Vapor Frac Mole Flow kmol/hr Mass Flow kg/hr Volume Flow cum/hr Enthalpy Gcal/hr Mass Flow kg/hr CO BMIMTF 2 N trace trace trace trace trace trace CH Mass Frac CO BMIMTF 2 N trace trace trace trace trace trace CH PPM PPM PPM PPM Mole Flow kmol/hr CO BMIMTF 2 N trace trace trace trace trace trace CH Mole Frac CO BMIMTF 2 N trace trace trace trace trace trace CH PPM PPM PPM
23 Table S13 Stream results of the flowsheet for IL-based Decarbonization (two single-stage) (raw gas V CO2 :V CH4 =60%:40%) ACIDGAS BMIMNTF2 GASIN GASOUT LEANOUT RICHOUT Temperature C Pressure bar Vapor Frac Mole Flow kmol/hr Mass Flow kg/hr Volume Flow cum/hr Enthalpy Gcal/hr Mass Flow kg/hr CO BMIMTF 2 N trace trace trace trace trace trace CH Mass Frac CO BMIMTF 2 N trace trace trace trace trace trace CH PPM PPM PPM PPM Mole Flow kmol/hr CO BMIMTF 2 N trace trace trace trace trace trace CH Mole Frac CO BMIMTF 2 N trace trace trace trace trace trace CH PPM PPM PPM
24 Table S14 Stream results of the flowsheet for IL-based Decarbonization (two single-stage) (raw gas V CO2 :V CH4 =80%:20%) ACIDGAS BMIMNTF2 GASIN GASOUT LEANOUT RICHOUT Temperature C Pressure bar Vapor Frac Mole Flow kmol/hr Mass Flow kg/hr Volume Flow cum/hr Enthalpy Gcal/hr Mass Flow kg/hr CO BMIMTF 2 N trace trace trace trace trace trace CH Mass Frac CO BMIMTF 2 N trace trace trace trace trace trace CH PPM PPB PPB PPB 945 PPM Mole Flow kmol/hr CO BMIMTF 2 N trace trace trace trace trace trace CH Mole Frac CO BMIMTF 2 N trace trace trace trace trace trace CH PPM PPM PPM
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