Ilconich, J. B.

Luebke, D. R.

Myers, C. R.

Pennline, H. W.

UNT Digital Library

Supported Ionic Liquid Membranes for Carbon Dioxide SeparationDavid Luebke, Jeffery Ilconich, Christina Myers, Henry PennlineOctober 17, 2006American Filtration & Separations Society2K-2571 GoalsCarbon Sequestration Programmatic Goal:Capture and secure 90% of CO2 emissions from new power plants with no more than 10% increase in the cost of energy services by 2012.Membrane Project Goal:Support the sequestration programmatic goal by developing membranes which can lower the costs associated with precombustion capture of CO2 from IGCC systems.SILM Study Goal:Develop CO2 selective supported ionic liquid membranes with sufficient permeability and selectivity to allow capture of CO2at an acceptably low cost.2K-2571 STACKMildGasCleanupWater-GasShiftGasTurbineFilterCoalWaterO2CO2MembraneGasifierColdGasCleanupPrecombustion CO2 Capture in IGCC2K-2571 Potential of Ionic Liquids• Negligible Vapor Pressure• Thermally Stable above 200oC• High CO2 Solubility Relative to H2, N2, and CH4NPCationsClCF3NSSCF3O OO ONO OOCN           CNNAnionsNNC6H132K-2571 Several Fabrication OptionsPorous SubstrateDense Substrate2K-2571 Selection of Support Material Significant• Suggested by Noble et al. as a useful support*• Tg ~ 210oC• Visible change when heated to 100oC in the presence of [hmim][Tf2N]• Membrane failure occurs at less than 50oC*Scovazzo et al. in: R. Rogers, K. Seddon (EDS.) Industrial Applications of Ionic Liquids, American Chemical Society Books, 2002, Chapter 6.PES Support-Supor®PSF Support-HT Tuffryn®• Unmodified Tg ~ 150oC• Membrane stable to 125oC2K-2571 Constant Pressure Flux MeasurementsFurnaceFeed Sweep andCarrier Gas(argon)GCCarrier GasRotometerRotometerP PT2K-2571 Support Failure Limits Performance110100001000100Selectivity3.12.72.3 2.5 2.9 3.31000/T K-1Y=6206e-0.6435xR2=0.9569Y=72571e-2.0902xR2=0.9994Y=0.1154e1.3483xR2=0.9954PermeabilityBarrer CO2He35oC50oC75oC125oC 100oC2K-2571 Other Mechanisms InconsistentOriginalMechanismPoreCollapseI.L.DegradationNewMedium2K-2571 Temperature oC50 75 100 125 150 175 200 225 250Heat Flow W/gPES without Ionic LiquidPES with Ionic LiquidDSC Confirms Large Tg Reduction for PES2K-2571 50 75 100 125 150 175 200 225 250Heat FlowW/gPSF without Ionic LiquidPSF with Ionic LiquidPSF Less AffectedTemperatureoC2K-2571 2.3 2.5 2.7 2.9 3.1 3.3 3.510000100010010Permeability Barrer75oC100oC 50oC 25oC125oCBaltus et al., Separation Science and Technology, 40 (2005) 525.Scovazzo et al., Journal of Membrane Science, 238 (2004) 57.CO2 Permeabilities Similar to Literature1000/T K-12K-2571 2.4 2.8 3.0 3.2 3.4 3.62.61.0E-61.0E-71.0E-51.0E-4Diffusivity cm2/s125oC 100oC 75oC 50oC 25oCMorgan et al., Ind. Eng. Chem. Res., 44 (2005) 4815.Shiflett and Yokozeki, Ind Eng. Chem. Res., 44 (2005) 4453.1000/TK-1CO2 Diffusivities Comparable to Literature2K-2571 He and H2 Results Similar11010000100010035oC50oC75oC100oC3.12.72.3 2.5 2.9 3.3Y=6206e-0.6435xY=37228e-1.7414XY=0.0902e1.303x1000/T K-1PermeabilityBarrerSelectivityCO2H22K-2571 110100010035oC50oC75oC100oC3.12.72.3 2.5 2.9 3.3Y=6206e-0.6435xY=37228e-1.7414XY=0.0902e1.303x1000/T K-1PermeabilityBarrerSelectivityCO2H2Commercial IL is Comparable2K-2571 100371003710037Temperature (oC)2.96.83.07.03.36.4Selectivity (CO2/H2)367109350121359136H2 Permeability (Barrer)106074210408401170817CO2Permeability (Barrer)Wet Gas MixtureDry Gas MixturePure GasEffect of H2O in Feed and Non-Ideality2K-2571 SILMs versus Polymers0.11101000.01 0.1 1 10 100 1000 10000Polymer Literature DataLin et al., Science 311 (2006) 639.SILMPermeability BarrerCO2/H2Selectivity2K-2571 Summary • Support selection in SILM is nontrivial.• Support performance is predictable by DSC analysis.• Current performance limited by support failure and IL blowout.• Ideal and non-ideal selectivities similar.• Performance not significantly impacted by a small amount of water in the feed.• Unoptimized SILMs are competitive with the best polymer membranes.• Industrially produced ILs of lower purity remain competitive.2K-2571 AcknowledgementsThe authors gratefully acknowledge the Brennecke and Maginn research groups at the University of Notre Dame.Their efforts in the synthesis and characterization of the ionic liquids along with their invaluable expertise in these areas have been very beneficial in the development of this exciting new technology. We look forward to continued fruitful collaboration.

Supported Ionic Liquid Membranes for Carbon Dioxide Separation

Luebke, David R.

Ilconich, Jeffery B.

Myers, Christina

Pennline, Henry W.

Supported Ionic Liquid Membranes for Carbon Dioxide SeparationDavid Luebke, Jeffery Ilconich, Christina Myers, Henry PennlineMay 9, 20065th Conference on Carbon Capture & Sequestration2K-2571 STACKMildGasCleanupWater-GasShiftGasTurbineFilterCoalWaterO2CO2MembraneGasifierColdGasCleanupPrecombustion CO2 Capture in IGCC2K-2571 Potential of Ionic Liquids• Negligible Vapor Pressure• Thermally Stable above 200oC• High CO2 Solubility Relative to H2, N2, and CH4NPCationsClCF3NSSCF3O OO ONO OOCN           CNNAnionsNNC6H132K-2571 Several Fabrication OptionsPorous SubstrateDense Substrate2K-2571 Selection of Support Material Significant• Suggested by Noble et al. as a useful support*• Tg ~ 210oC• Visible change when heated to 100oC in the presence of [hmim][Tf2N]• Membrane failure occurs at less than 50oC*Scovazzo et al. in: R. Rogers, K. Seddon (EDS.) Industrial Applications of Ionic Liquids, American Chemical Society Books, 2002, Chapter 6.PES Support-Supor®PSF Support-HT Tuffryn®• Unmodified Tg ~ 150oC• Membrane stable to 125oC2K-2571 Constant Pressure Flux MeasurementsFurnaceFeed Sweep andCarrier Gas(argon)GCCarrier GasRotometerRotometerP PT2K-2571 Support Failure Limits Performance110100001000100Selectivity3.12.72.3 2.5 2.9 3.31000/T K-1Y=6206e-0.6435xR2=0.9569Y=72571e-2.0902xR2=0.9994Y=0.1154e1.3483xR2=0.9954PermeabilityBarrer CO2He35oC50oC75oC125oC 100oC2K-2571 Other Mechanisms InconsistentOriginalMechanismPoreCollapseI.L.DegradationNewMedium2K-2571 Temperature oC50 75 100 125 150 175 200 225 250Heat Flow W/gPES without Ionic LiquidPES with Ionic LiquidDSC Confirms Large Tg Reduction for PES2K-2571 50 75 100 125 150 175 200 225 250Heat FlowW/gPSF without Ionic LiquidPSF with Ionic LiquidPSF Less AffectedTemperatureoC2K-2571 2.3 2.5 2.7 2.9 3.1 3.3 3.510000100010010Permeability Barrer75oC100oC 50oC 25oC125oCBaltus et al., Separation Science and Technology, 40 (2005) 525.Scovazzo et al., Journal of Membrane Science, 238 (2004) 57.Permeabilities Similar to Literature1000/T K-12K-2571 2.4 2.8 3.0 3.2 3.4 3.62.61.0E-61.0E-71.0E-51.0E-4Diffusivity cm2/s125oC 100oC 75oC 50oC 25oCMorgan et al., Ind. Eng. Chem. Res., 44 (2005) 4815.Shiflett and Yokozeki, Ind Eng. Chem. Res., 44 (2005) 4453.1000/TK-1Diffusivities Comparable to Literature2K-2571 2.6 2.8 3.0 3.12.92.7 3.33.210100001000100PermeabilityBarrer100oC 75oC 50oC 35oCCO2HeH21000/TK-1Separation from H2 Favorable2K-2571 2.6 2.8 3.0 3.12.92.7 3.33.2100oC 75oC 50oC 35oC10987654321CO2/H2CO2/He1000/TK-1SelectivityTemperature Dependence Similarity2K-2571 100371003710037Temperature (oC)2.96.83.07.03.36.4Selectivity (CO2/H2)367109350121359136H2 Permeability (Barrer)106074210408401170817CO2Permeability (Barrer)Wet Gas MixtureDry Gas MixturePure GasH2O in Feed and Non-Ideality Insignificant2K-2571 SILM’s versus Polymers0.11101000.01 0.1 1 10 100 1000 10000Polymer Literature DataLin et al., Science 311 (2006) 639.SILMPermeability BarrerCO2/H2Selectivity2K-2571 Summary • Support selection in SILM is nontrivial.• Support performance is predictable by DSC analysis.• Current performance limited by support failure and IL blowout.• Ideal and non-ideal selectivities similar.• Performance not significantly impacted by a small amount of water in the feed.• Unoptimized SILM’s are competitive with the best polymer membranes.2K-2571 AcknowledgementsThe authors gratefully acknowledge the Brennecke and Maginn research groups at the University of Notre Dame.Their efforts in the synthesis and characterization of the ionic liquids along with their invaluable expertise in these areas have been very beneficial in the development of this exciting new technology. We look forward to continued fruitful collaboration.

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Supported Ionic Liquid Membranes for Carbon Dioxide Separation

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