Novel Landfill-Gas-to-Biomethane Route Using a Gas–Liquid Membrane Contactor for Decarbonation/Desulfurization and Selexol Absorption for Siloxane Removal
Abstract
:1. Introduction
1.1. Landfill-Gas Decarbonation: Advantages of Gas–Liquid Membrane Contactors
1.2. GLMC Modeling for Landfill-Gas/Biogas Decarbonation
1.3. GLMC Modeling in Process Simulators
1.4. Siloxane Removal from Landfill-Gas: The Advantages of Selexol Absorption
1.5. The Present Work
2. Methods
2.1. GLMC-UOE Development
2.1.1. Element Mass Balances
2.1.2. Element Energy Balances
2.1.3. Element Pressure Drop
2.1.4. Algorithm to Solve the Countercurrent GLMC Model (GLMC-CCC-D)
2.1.5. Algorithm to Solve the Parallel-Contact GLMC (GLMC-PC-D)
2.1.6. GLMC-UOE Validation
2.2. Landfill-Gas Composition
2.3. Landfill-Gas-to-Biomethane Simulation Assumptions
2.4. Landfill-Gas-to-Biomethane Process
2.4.1. Landfill-Gas Pre-Processing and Compression
2.4.2. Intensified GLMC Decarbonation/Desulfurization with Pressurized Water
2.4.3. Siloxane Removal via DEPG Absorption
3. Landfill-Gas-to-Biomethane Process: Results and Discussion
3.1. Landfill-Gas Decarbonation/Desulfurization Results
3.2. Siloxane Separation, Process Waste, and Power/Utilities Consumption
4. Conclusions
Supplementary Materials
Author Contributions
Funding
Data Availability Statement
Conflicts of Interest
Abbreviations
Nomenclature
HFM-side and shell-side flow-section areas (m2) | |
GLMC module transfer area (m2) | |
, | Shell internal diameter, HFM-side hydraulic diamter, and shell-side hydraulic diameter (m) |
Internal/external HFM diameters (m) | |
L/V species k fugacities at element n (bar) | |
Logarithmic mean of k transmembrane fugacity difference at element n (bar) | |
L/V kth partial molar enthalpies at element n (kJ/kmol) | |
L/V molar enthalpies at element n (kJ/kmol) | |
Shell-side and HFM-side head losses for element n (Pa) | |
Vector of species L molar flowrates leaving element n (mol/s) | |
Number of discretized GLMC elements; number of HFMs per module | |
Transmembrane k transfer rate (mol/s) in element n and number of modules | |
Cente–-center distance of adjacent HFMs (m) | |
L/V pressures of element n (bar) | |
Logarithmic mean transmembrane temperature difference at element n (K) | |
L/V temperatures of element n (K) | |
External/internal GLMC heat transfer coefficients (kJ/(h.m2.K)) | |
Vector of species V molar flowrates leaving element n (mol/s) | |
L/V axial velocities at element n (m/s) | |
L and V species k mol fraction | |
, z | GLMC length; GLMC axial position (m) |
Greek Symbols | |
Packing ratio; Kozeny factor | |
L/V dynamic viscosities at element n (Pa.s) | |
Transmembrane k mass transfer coefficient (mol/(s.bar.m2)) | |
L/V molar densities at element n (kmol/m3) |
Appendix A. GLMC-PC-D Model Validation
Item | Value | Item | Value | Item | Value | Item | Value |
---|---|---|---|---|---|---|---|
0.8 m | 0.502 mm | mol/(s.bar.m2) | mol/(s.bar.m2) | ||||
2 m | mol/(s.bar.m2) | mol/(s.bar.m2) | |||||
Volume | 1.005 m3 | 6901.4 m2 | mol/(s.bar.m2) | mol/(s.bar.m2) | |||
40 | 27 °C | mol/(s.bar.m2) | mol/(s.bar.m2) | ||||
0.5 mm | 5 W/(m2.K) | mol/(s.bar.m2) | 2 W/(m2.K) |
Solvent Inlet | CO2-Rich NG Inlet | Treated Gas [54] | Treated-Gas GLMC-PC-D | |
---|---|---|---|---|
P (bar) | 5.0 | 50.0 | 49.85 | 49.85 |
T (°C) | 26.85 | 26.85 | 38.80 | 39.77 |
MMNm3/d | - | 1.0 | 0.830 | 0.829 |
kg/h | 17,651 | - | - | - |
CO2 (%mol) | 0 | 10.19 | 3.50 | 3.36 |
CH4 (%mol) | 0 | 73.22 | 76.5 | 76.41 |
C2H6 (%mol) | 0 | 9.09 | 11.00 | 10.97 |
C3H8 (%mol) | 0 | 4.25 | 5.10 | 5.14 |
C4H10 (%mol) | 0 | 1.78 | 2.20 | 2.15 |
C5H12 (%mol) | 0 | 1.47 | 1.80 | 1.77 |
H2O (%mol) | 60 | 0 | 0 | 0.20 |
MEA (%mol) | 20 | 0 | 0 | |
MDEA (%mol) | 20 | 0 | 0 |
Appendix B. GLMC-PC-D Model Asymptotic Validation with P-H Flash
CO2-Rich Solvent P-H Flash | CO2-Rich Solvent GLMC-PC-D | Treated-Gas P-H Flash | Treated-Gas GLMC-PC-D | |
---|---|---|---|---|
P (bar) | 50.0 | 50.0 | 50.0 | 50.0 |
T (°C) | 65.90 | 65.90 | 65.90 | 65.90 |
kmol/h | 440.4 | 439.3 | 1796.4 | 1797.5 |
kg/h | 20,629 | 20,605 | 39,302 | 39,326 |
CO2 (%mol) | 15.94 | 15.99 | 6.64 | 6.64 |
CH4 (%mol) | 0.31 | 0.12 | 75.74 | 75.74 |
C2H6 (%mol) | 0.06 | 0.01 | 9.40 | 9.40 |
C3H8 (%mol) | 0.02 | 4.40 | 4.40 | |
C4H10 (%mol) | 0.01 | 1.52 | 1.52 | |
C5H12 (%mol) | 0.01 | 1.84 | 1.84 | |
H2O (%mol) | 49.43 | 49.58 | 0.46 | 0.46 |
MEA (%mol) | 17.11 | 17.15 | ||
MDEA (%mol) | 17.11 | 17.15 |
Appendix C. GLMC-CCC-D Asymptotic Validation with an Adiabatic Absorption Column
Item | CO2-Rich Solvent Absorber | CO2-Rich Solvent GLMC-CCC-D | Treated-Gas Absorber | Treated-Gas GLMC-CCC-D |
---|---|---|---|---|
P (bar) | 50.0 | 50.0 | 50.0 | 50.0 |
T (°C) | 26.53 | 40.12 | 91.75 | 89.87 |
kmol/h | 444.0 | 456.9 | 1792.8 | 1779.9 |
kg/h | 21,182 | 21,185 | 38,749 | 38,746 |
CO2 (%mol) | 20.09 | 17.59 | 5.60 | 6.13 |
CH4 (%mol) | 0.11 | 0.11 | 75.93 | 76.48 |
C2H6 (%mol) | 0.04 | 9.42 | 9.50 | |
C3H8 (%mol) | 0.02 | 4.41 | 4.44 | |
C4H10 (%mol) | 0.01 | 1.52 | 1.54 | |
C5H12 (%mol) | 0.01 | 1.86 | 1.86 | |
H2O (%mol) | 45.81 | 49.32 | 1.26 | 0.05 |
MEA (%mol) | 16.95 | 16.49 | ||
MDEA (%mol) | 16.96 | 16.49 |
Appendix D. GLMC-CCC-D Model Validation: Water Solvent GLMC
Biomethane [47] | Biomethane GLMC-CCC-D | Off Gas [47] | Off-Gas GLMC-CCC-D | |
---|---|---|---|---|
P (bar) | -- | 7.996 | -- | 0.6831 |
T (°C) | 15 | 15.25 | 15 | 18.37 |
Nm3/h | 33.61 | 33.73 | 140.88 | 141.55 |
CO2 (%mol) | 2 | 2 | 13.4 | 13.7 |
CH4 (%mol) | 98 | 98 | 2.2 | 2.2 |
N2 (%mol) | 0 | 0 | 84.3 | 84.1 |
Process: General Results | ||||
Belaissaoui and Favre [47] | GLMC-CCC-D | |||
Liquid Pressure Drop (bar) | 2.43 | 2.47 | ||
CO2 %Removal | 96.65 | 96.53 | ||
CH4 %Loss | 8.7 | 8.5 | ||
CO2-Rich Solvent Temperature (°C) | 15 | 15.26 | ||
Regenerated Solvent Temperature (°C) | 15 | 15.03 |
Appendix E. GLMC Internal Heat Transfer Coefficient for Landfill-Gas Purification
Item | CO2-Rich Water Absorber | CO2-Rich Water GLMC-CCC-D | Treated-Gas Absorber | Treated-Gas GLMC-CCC-D |
---|---|---|---|---|
P (bar) | 7.1 | 6.664 | 7.0 | 6.998 |
T (°C) | 15.37 | 15.37 | 15.02 | 15.08 |
MMNm3/d | - | - | 0.252957 | 0.253672 |
kg/h | 7,276,541 | 7,276,586 | - | - |
CH4 (%mol) | 0.01 | 0.01 | 99.10 | 99.10 |
CO2 (%mol) | 0.09 | 0.09 | 0.64 | 0.13 |
H2S (ppm-mol) | ||||
H2O (%mol) | 99.90 | 99.90 | 0.26 | 0.26 |
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Name | ID | Formula | Molar Mass (g/mol) | Content (mg/Nm3) |
---|---|---|---|---|
Hexamethyl-disiloxane | L2 | C6H18OSi2 | 162.38 | 6.07 |
Octamethyl-trisiloxane | L3 | C8H24O2Si3 | 236.53 | - |
Decamethyl-tetrasiloxane | L4 | C10H30O3Si4 | 310.69 | 0.04 |
Dodecamethyl-pentasiloxane | L5 | C12H36O4Si5 | 384.84 | - |
Tetradecamethyl-hexasiloxane | L6 | C14H42O5Si6 | 458.99 | 0.01 |
Hexamethyl-cyclotrisiloxane | D3 | C6H18O3Si3 | 222.46 | 0.49 |
Octamethyl-cyclotetrasiloxane | D4 | C8H24O4Si4 | 296.62 | 12.53 |
Decamethyl-cyclopentasiloxane | D5 | C10H30O5Si5 | 370.77 | 4.73 |
Dodecamethyl-cyclohexasiloxane | D6 | C12H36O6Si6 | 444.93 | 0.33 |
Trimethyl-silanol | TMS | C3H10OSi | 90.20 | - |
Total (ppm-mol) | 2.14 |
Topic | Description |
---|---|
Thermodynamic Modeling | Landfill-Gas Compression, CO2/H2S Separation, Siloxanes Separation: HYSYS Acid-Gas Physical-Solvents Package; CO2-to-EOR: PR-EOS; Cooling-Water(CW)/Chilled-Water(ChW)/LPS,MPS: HYSYS ASME-Steam-Table; |
Landfill-Gas | 0.5 MMNm3/d; T = 30 °C; P = 1 bar; Mol = 27.73 g/mol; CH4 = 55.7 %mol; CO2 = 40 %mol; H2OSaturation = 4.28 %mol; H2S = 150 ppm-mol; Siloxanes: Table 1. |
Biomethane | CH4 ≥ 85 %mol; CO2 ≤ 3 %mol; H2S ≤ 10 mg/Nm3; Siloxanes ≤ 0.03 mg/Nm3 [19,85,86] |
GLMC Module [47] | HFM: Polyphenylene-Oxide (Parker P-240); ; ; HFM-Side:Landfill-Gas; Shell-Side:Water; = 0.36 m; Packing-Ratio: = 0.5; ; GLMC-Absorber: ; GLMC-Stripper: ; |
GLMC Modeling | ;
; === mol/(s.bar.m2);= mol/(s.bar.m2); ; Capture-Ratio = 443.41 kgH2O/kgCO2; {TS} = {CO2, H2S, CH4, H2O}; GLMC-CCC-D: Countercurrent-Contact Distributed-Model (Section 2.1); GLMC-PC-D: Parallel-Contact Distributed-Model (Section 2.1). |
High-Pressure CO2/H2S Reboilered Stripper | Feed[H2O/CO2/H2S] = 7,275,950 kg/h; ; Feed-Stage = 5; ; ; Condenser: Total-Reflux; Reboiler: Kettle (MPS); Reflux-RatioTop = 721.6. |
DEPG Absorber | Solvent: 35.06 kmol/h; DEPG = 98.4 %w/w; H2O = 1.6 %w/w;; ; = 6.995 bar; = 17.29 °C; StagesTheoretical = 20. |
DEPG Reboilerd Stripper | Feed: 36.85 kmol/h; = 1.17 bar; = 162.7 °C; StagesTheoretical = 10; Feed-Stage = 5; = 1.1 bar; = 88.72 °C; = 1.2 bar; = 175 °C; Condenser: Total-Reflux; Reboiler: Kettle (LPS); Reflux-RatioTop = 100. |
Saturated-Steam [87] | Low-Pressure-Steam (LPS): P = 14.3 bar, T = 196 °C; Medium-Pressure-Steam (MPS): P = 42.5 bar, T = 254 °C. |
Compressors | Adiabatic-Efficiency = 75%; Compression-RatioStage = 3 (Landfill-Gas); Compression-RatioStage = 2.25 (CO2-to-EOR). |
Pumps | Adiabatic-Efficiency = 75%. |
Intercoolers | TGas-Out = 40 °C; ΔPGas = 0.5 bar. |
Exchangers | . |
Cooling-Water | . |
Chilled-Water | . |
Streams | Fugacity | CO2 | CH4 | H2S | H2O |
---|---|---|---|---|---|
Inlets | (bar) | 2.812 | 3.989 | 0.074 | |
(bar) | 0 | 0 | 0.017 | ||
GLMC-CCC-D Outlets | (bar) | 0.203 | 6.669 | 0.019 | |
(bar) | 1.190 | 3.899 | 0.018 | ||
GLMC-PC-D Outlets | (bar) | 0.989 | 5.876 | 0.018 | |
(bar) | 0.977 | 5.120 | 0.017 |
Landfill-Gas Inlet | Water Inlet | GLMC-CCC-D Landfill-Gas Outlet | GLMC-CCC-D Water Outlet | GLMC-PC-D Landfill-Gas Outlet | GLMC-PC-D Water Outlet | |
---|---|---|---|---|---|---|
P (bar) | 7.0 | 7.0 | 6.995 | 6.213 | 6.996 | 6.211 |
T (°C) | 40.00 | 15.00 | 17.29 | 15.37 | 21.11 | 15.32 |
MMNm3/d | 0.483961 | - | 0.261854 | - | 0.286783 | - |
kg/h | - | 7,259,307 | - | 7,275,950 | - | 7,273,439 |
H2O (%mol) | 1.11 * | 100 | 0.29 | 99.90 | 0.28 | 99.91 |
CH4 (%mol) | 57.55 | 96.71 | 0.01 | 85.14 | 0.02 | |
CO2 (%mol) | 41.32 | 3.0 | 0.09 | 14.59 | 0.07 | |
H2S (ppm-mol) | 154.94 | 4.94 | 0.34 | 21.53 | 0.32 | |
D3 (ppb-mol) # | 50.97 | 0 | 94.21 | 0 | 86.02 | 0 |
D4 (ppb-mol) # | 977.59 | 0 | 1806.79 | 0 | 1649.73 | 0 |
D5 (ppb-mol) # | 1.16 | 0 | 2.15 | 0 | 1.96 | 0 |
D6 (ppb-mol) # | 12.46 | 0 | 23.03 | 0 | 21.03 | 0 |
L2 (ppb-mol) # | 865.09 | 0 | 1598.87 | 0 | 1459.89 | 0 |
L4 (ppb-mol) # | 2.84 | 0 | 5.24 | 0 | 4.79 | 0 |
L6 (ppb-mol) # | 0.50 | 0 | 0.93 | 0 | 0.85 | 0 |
Siloxanes (ppb-mol) # | 1910.61 | 0 | 3531.22 | 0 | 3224.27 | 0 |
Final Results: Gas-to-Solvent CO2/H2S %Recoveries and Gas-to-Solvent CH4 %Loss | ||||||
GLMC Battery | %Recovery CO2 | %Recovery H2S | %Loss CH4 | |||
GLMC-PC-D | 79.08 | 91.77 | 12.33 | |||
GLMC-CCC-D | 96.08 | 98.28 | 9.07 |
Inlet Landfill-Gas | Outlet Landfill-Gas | Stripper Top Gas | Excess Water | |
---|---|---|---|---|
H2O (kmol/h) | 10.03 | 1.43 | 1.28 | 7.32 |
CH4 (kmol/h) | 518.05 | 471.05 | 47.00 | |
CO2 (kmol/h) | 372.00 | 14.59 | 357.41 | |
H2S (kmol/h) | 0.1395 | 0.0024 | 0.1371 | |
High-Pressure CO2/H2S Stripper—Water Regeneration | ||||
Stripper Top Gas | Lean Water | |||
P (bar) | 30.0 | 30.2 | ||
T (°C) | 40.0 | 233.8 | ||
kmol/h | 405.82 | 402,960.11 | ||
MMNm3/d | 0.218 | - | ||
H2O (%mol) | 0.31 | 100 | ||
CH4 (%mol) | 11.58 | |||
CO2 (%mol) | 88.07 | |||
H2S (ppm-mol) | 337.78 |
Biomethane Outlet | Absorber Rich DEPG | Stripper Top Gas | Lean DEPG | |
---|---|---|---|---|
P (bar) | 6.9 | 6.995 | 1.1 | 1.2 |
T (°C) | 15.84 | 19.35 | 88.72 | 175 |
kmol/h | 485.28 (0.26 MMNm3/d) | 36.86 | 1.80 | 35.06 |
DEPG (%mol) | 75.98 | 79.87 | ||
H2O (%mol) | 0.31 | 22.12 | 61.09 | 20.13 |
CH4 (%mol) | 96.97 | 1.24 | 25.54 | |
CO2 (%mol) | 2.96 | 0.65 | 13.26 | |
H2S (ppm-mol) | 4.36 (6.7 mg/Nm3) | 7.77 | 159.44 | |
D3 (ppm-mol) | 1.25 | 25.6 | ||
D4 (ppm-mol) | 23.9 | 490 | ||
D5 (ppm-mol) | 0.00145 | 12.2 | 12.8 | |
D6 (ppm-mol) | 0.00025 | 57.2 | 5.09 | 59.9 |
L2 (ppm-mol) | 21.1 | 434 | ||
L4 (ppm-mol) | 0.00001 | 0.1935 | 1.59 | 0.122 |
L6 (ppm-mol) | 0.0123 | 0.253 | ||
Siloxanes (ppm-mol) | 0.0017 (0.029 mg/Nm3) | 116 | 957 | 72.8 |
Inlet Landfill-Gas | Outlet Biomethane | Top-Gas Stripper | DEPG Make-Up | |
---|---|---|---|---|
DEPG (kmol/h) | 0 | |||
H2O (kmol/h) | 1.43 | 0.33 | 1.10 | 0 |
CH4 (kmol/h) | 471.05 | 470.59 | 0.46 | - |
CO2 (kmol/h) | 14.59 | 14.35 | 0.24 | - |
H2S (kmol/h) | 0.0024 | 0.0021 | 0.0003 | - |
Siloxanes (kmol/h) | - | |||
Process Wastes | Power and Utilities Consumption | |||
Residual Gas | Residual Water | Consumption | ||
kmol/h | 0.76 | 1.04 | Power | 9.41 MW |
DEPG (%mol) | 0 | 0 | Chilled Water | 16,461 t/h |
H2O (%mol) | 7.44 | 99.99 | Cooling Water | 225,507 t/h |
CH4 (%mol) | 60.77 | 0.00124 | LPS | 4 t/h |
CO2 (%mol) | 31.53 | 0.01 | MPS | 8604 t/h |
H2S (ppm-mol) | 378.76 | 0.45 | ||
Siloxanes (ppm-mol) | 2200 | 7.71 |
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© 2024 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).
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da Cunha, G.P.; de Medeiros, J.L.; Araújo, O.d.Q.F. Novel Landfill-Gas-to-Biomethane Route Using a Gas–Liquid Membrane Contactor for Decarbonation/Desulfurization and Selexol Absorption for Siloxane Removal. Processes 2024, 12, 1667. https://doi.org/10.3390/pr12081667
da Cunha GP, de Medeiros JL, Araújo OdQF. Novel Landfill-Gas-to-Biomethane Route Using a Gas–Liquid Membrane Contactor for Decarbonation/Desulfurization and Selexol Absorption for Siloxane Removal. Processes. 2024; 12(8):1667. https://doi.org/10.3390/pr12081667
Chicago/Turabian Styleda Cunha, Guilherme Pereira, José Luiz de Medeiros, and Ofélia de Queiroz F. Araújo. 2024. "Novel Landfill-Gas-to-Biomethane Route Using a Gas–Liquid Membrane Contactor for Decarbonation/Desulfurization and Selexol Absorption for Siloxane Removal" Processes 12, no. 8: 1667. https://doi.org/10.3390/pr12081667