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US 8,128,735B1 12 PROCESS FOR CO2 CAPTURE USING ZEOLITES FROM HIGH PRESSURE AND MODERATE TEMPERATURE GAS STREAMS STATEMENT OF GOVERNMENTAL SUPPORT The United States Government has rights in this invention pursuanttotheemployer-employeerelationshipoftheGov ernment to the inventors as US. Department of Energy employeesattheNationalEnergyTechnologyLaboratory. TECHNICAL FIELD C.Thistemperaturelimitationisfurthercomplicatedbythe heat of adsorption associated With Zeolites, generating the tendencyforadsorptionbedtemperaturestoincreaseconsid erably, and often necessitating adsorption bed cooling With external refrigeration to maintain the gas at temperatures beloW 40° C. This places signi?cant limitation on the appli cation of Zeolites for adsorption of carbon dioxide at high temperature, Which is becoming increasingly signi?cant in ?elds such as emission control of fossil-fueled poWer sys tems, natural gas treatments, puri?cation of hydrocarbons, andproductionofhydrogengas,amongothers.Intheseappli cations and others, itWould be advantageous to provide a cycle Where Zeolite adsorbents could be utiliZed in a manner preserving the adsorption capacity at higher temperatures, such that parasitic external refrigeration loads could be reducedoreliminated.Suchacapabilitycouldhaveparticular importforgaseousstreamseparationintheproductionofH2 from shifted syngas using a Water-gas-shift reactor, Where A methodforseparatingCO2 fromagasstreamcomprised ofCO2 andothergaseousconstituentsusingaZeolitesorbent inasWing-adsorptionprocess,producingahightemperature CO2 stream at a higher CO2 pressure than the input gas stream.ThemethodutiliZesCO2 desorptioninaC02 atmo sphereandeffectivelyintegratesheattransfersforoptimiZes anyrequirementtomaintaintemperatureoftheadsorbentbed overalle?iciency.H2Oadsorptiondoesnotprecludeeffective20 operationofthesorbent.The cyclemay beincorporatedinan IGCC fore?icientpre-combustionCO2 capture.A particular application operates on shifted syngas at a temperature exceeding 200° C. and produces a dry CO2 stream at loW temperatureandhighCO2pressure,greatlyreducingany25 compression energy requirements Which may be subse quentlyrequired. BACKGROUND OF THE INVENTION 30 TheemissionofCO2 frompoWerplantshasbeenidenti?ed as a factor potentially resulting in long-term environmental problems. Consequently, separation of CO2 from gaseous streams utiliZing adsorption of gases and vapors by microporoussolidshasattractedattention,becauseofits35 greatpracticalimportanceinthe?eldsofgasseparationand gas puri?cation. Certain technologies based on the CO2 adsorption/desorptionbyusingnaturalandsyntheticZeolites are among the most effective methods. beloW20°C.leviessigni?cantrefrigerationrequirements. Such a capability has further advantage When separation operations occur priorto combustion ofa non-adsorbed com ponent, so that refrigeration requirements have a direct impact on the subsequent ef?ciency of the combustion. For example,theseparationofCO2andH2fromaWater-gasshift (WGS) reactor in preparation for H2 combustion in an Inte gratedGasi?cationCombinedCycle(IGCC)plant. ItisknoWn thattheadsorptionofsome Zeolitesincreasesas thepressureoftheadsorbentbedinincreasedforsome appli cations.Seee.g.,SiriWardaneetal,“AdsorptionofCO2,N2, and02onnaturalZeolites,”Energy& Fuels,Vol.17(2003), discussingtheadsorptionofcertainZeolitesattemperatures of 25° C. and pressures up to 300 psig. See also SiriWardane etal,“AdsorptionofCO2 onZeolitesatModerateTempera tures,”Energy&Fuels,Vol.19(2005),discussingtheadsorp tion of certain Zeolites at temperatures up to 120° C. and pressures up to 300 psig, and regeneration at 300° C. under an N2atmosphere.Generallyspeaking,investigationsofdiverse ZeoliteshaveindicatedthatthecapacityforCO2 adsorptionis enhancedWhenthepartialpressureofCO2increases.See Bonenfant etal,“Advances inprincipal factors in?uencing carbon dioxide adsorption on Zeolites,” Sci. Technol. Adv. Mater 9(2008).AsWing-adsorptioncycleforCO2 separation using Zeolites that takes advantage of the propensity for increasedadsorptionaspressureincreasesWouldalloWZeo lite use at higher temperatures, further reducing or eliminat ing parasitic external refrigeration loads. Additionally, and signi?cantly, such a sWing-adsorption process Would have great bene?t if desorption could occur at the higher pressure andproduceahigherpressureCO2productstream,reducing Generally,tWomethodsareusedforCO2adsorption/des 40 orptionutiliZingZeoliteadsorbentsforCO2 separation:Tem perature SWing Adsorption (TSA) and Pressure SWing Adsorption (PSA). In each of these techniques, a bed of ZeoliteadsorbentisexposedtoaHow offeedairundertem peratureandpressureconditionsalloWingtheZeoliteadsor 45 bent to adsorb some portion of the carbon dioxide and Water vapor present in the feed air. This exposure continues for a periodoftime,andtypicallyceasespriortobreak-throughof carbon dioxide and Water in the exiting treated feed air. Fol loWingthisexposure,theHowoffeedairisceasedandthe50 adsorbentisregenerated.InatemperaturesWingadsorber,the compressionburdensWhichmightexistinsequestrationand carbondioxideandWateraredrivenofffromtheadsorbentby storageoperations. heatingtheadsorbentintheregenerationphase.Inapressure sWingadsorber,thepressureoftheregenerationgasisloWer thanthatofthefeedgasandthechangeinpressureisusedto 55 remove the carbon dioxide and Water from the adsorbent. There has been extensive research on the equilibrium of carbon dioxide on Zeolite adsorbent materials at ambient temperature and atmospheric pressure. It is established that Zeolitesef?cientlyremovecarbondioxideandWatervapor 60 from air streams at loW temperatures, i.e., temperatures of about 40° C. or loWer, because itmore strongly adsorbs these components thanitadsorbs nitrogen, oxygen orargon. HoW ever,atloWerpressures,thecarbondioxideadsorptioncapac ityofZeolitesgenerallydiminishrapidlyasthetemperature 65 ofthegasbeingseparatedincreases,andtheseparationpro cess can become infeasible at temperatures above about 40° Further,inCO2 separationforthepurposeofstorageand sequestration,purityoftheCO2 productstreamisofpara mountimportance.Often,insWing-adsorptioncyclesusing ZeolitesforCO2 separation,thehighertemperatureorloWer pressure regeneration must be assisted by the use of an inert regeneration gas to strip the adsorbed carbon dioxide and Waterfromtheadsorbent.TypicalapproachesutiliZeN2,He, orsomeportionofthepost-adsorptionfeedgas.Seee.g.,US. Pat. No. 5,968,234, issued to Midgett, issued Oct. 19, 1999; see also US. Pat. No. 5,855,650, issued to Kalbassi et al, issued Jan. 5, 1999, among others. The use of regeneration gas often increases the recovery of CO2 in Zeolite based sWing-adsorptionprocesses,hoWeverthepracticeinherently dilutes the recovered CO2 stream. In applications Where purityofthegeneratedCO2 streamisdesired,suchasinCO2PDF Image | PROCESS FOR CO2 CAPTURE USING ZEOLITES
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