BTF系统处理硫化氢废气工程设计外文参考文献译文及原文.doc

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BTF系统处理硫化氢废气工程设计外文参考文献译文及原文.doc

本科毕业设计(论文)

外文参考文献译文及原文

学院:

环境科学与工程学院

专业:

环境工程

年级班别:

2004级

(1)班

学号:

3104008168

学生姓名:

谢辉

指导教师:

陈凡植教授

2008年6月11日

1

Biologicalsweeteningofenergygasesmimicsinbiotricklingfilters

MarcFortunya,c,JuanA.Baezaa,XavierGamisansb,CarlesCasasa,JavierLafuentea,

MarcA.Deshussesc,*,DavidGabriela,1

aDepartmentofChemicalEngineering,UniversitatAuto`nomadeBarcelona,EdificiQ,CampusdeBellaterra,08193Bellaterra,Barcelona,Spain

bDepartmentofMiningEngineeringandNaturalResources,UniversitatPolite`cnicadeCatalunya,Manresa,Spain

cDepartmentofChemicalandEnvironmentalEngineering,UniversityofCalifornia,Riverside,CA92520,UnitedStates

Received25July2007;receivedinrevisedform27October2007;accepted29October2007

Availableonline21December2007

Abstract

Removalofhydrogensulfidefromwasteandenergy-richgasesisrequired,notonlybecauseofenvironmentalhealthandsafetyreasons,butalsobecauseofoperationalreasonsifsuchgaseshavetobeusedforenergygeneration.Abiotricklingfilterfortheremovalofultra-highconcentrationsofH2Sfromoxygen-poorgasesisproposedandstudiedinthiswork.Twolaboratory-scalebiotricklingfilterswereusedtostudythestartupperiodandtodeterminethelong-termperformanceofthegassweeteningprocess.TheinletH2Sconcentrationrangedfrom900to12000ppmvandtwodifferentpackingmaterialswereinvestigated.TherewasnotoxicityeffectobservedevenatathehighestH2Sconcentration,andmaximumeliminationcapacitiesof280and250gH2Sm-3h-1wereobtainedatgascontacttimesof167and180s,respectively.Elementalsulfurandsulfatewerefoundtobethemostabundantend-productsofthebiologicaloxidationofsulfidewhenoperatedundermicroaerophilicconditions.Thebiotricklingfilterwasabletoquicklyrecoveritsnominalperformanceafterdifferentloadincreasesandsystemshutdownssimulatingfieldoperation.Theresultsreportedhereshowthatbiotreatmentcanbeaninterestingalternativetoconventionalgassweeteningsystemsnormallyusedforsuchapplications.

Keywords:

Hydrogensulfide;Gassweetening;Biotricklingfilter;Desulfurization;Fuelgas;Biogas

1.Introduction

Hydrogensulfideisacommonreducedsulfurcompoundfoundinseveralindustrialwastegases.Itiseasilyrecognizablebyitsoffensiverotteneggsodor.However,odornuisanceisnotthemainissueinenergy-richgasessuchasbiogasfromanaerobicdigesterswhichmaycontainH2Sconcentrationsexceeding500ppmvandupto20000ppmv(2%v/v)(WoodcockandGottlieb,2004).Insuchcases,H2Sremoval,oftencalledgassweetening,isnecessarytoavoidcorrosionofcombustionenginesandSOxgenerationinthefluegases.Thus,removalofH2Sfromwasteandenergy-richgasesisrequired,notonlyforenvironmentalhealthandsafetyreasonsbutalsoforoperationalreasons.

Sofar,themostcommonlyusedtreatmenttechnologyforH2Sremovalisselectiveabsorptioninaminessuchasdiglycolamine,monoethanolamine,methyldiethanolamineorothercompoundsthathaveahighaffinityforH2S(WoodcockandGottlieb,2004).Althoughtheseprocesseshavebeenextensivelyandsuccessfullyapplied,theyhavemanydrawbackssuchashighenergyandoperatingcostsduetotheregenerationoftheabsorbentphase.Inthiscontext,biologicalprocessesforairpollutioncontrolaregainingpopularity(Deshusses,1997;Devinnyetal.,1999;KennesandVeiga,2001)buthavenotyetbeengenerallyappliedtotreatmentofH2Sinenergy-richgases.

BiologicalH2Sutilizationasenergysourceforlithoautotrophicorganismsisawell-knownprocessthatcanbedescribedwiththefollowingoverallreactions(Eqs.

(2),(3)).Notethatoxidationtoelementalsulfurcanonlyhappenunderoxygenlimitedconditions,andthatexcessoxygenisrequiredfortheformationofsulfate(Kuenen,1975;WoodcockandGottlieb,2004).

Biofilters,bioscrubbersandbiotricklingfiltershavebeenproventobeasuitable,environmentallyfriendlyandcosteffectivealternativeforwastegastreatment,especiallyforthetreatmentoflowconcentrationsofH2S(YangandAllen,1994;Devinnyetal.,1999;GabrielandDeshusses,2003a;KimandDeshusses,2005).However,therehasbeenlimitedsuccessindealingwithhighconcentrationsofH2S(>1000ppmv)usingbiofilters,biotricklingfiltersandbioscrubbersandonlyfewindustrialprocesseshavebeenfullydevelopedforsuchapplication.Amongthem,theThiopaqprocess(Paques,TheNetherlands),andtheBiopuricprocess(Biothane,USA)aretheonlyonesspecificallydevelopedfortheremovalofhighconcentrationsofH2Sfrombiogasorfuelgas.TheThiopaqprocessisatwo-reactorsystemconsistingofaconventionalcausticscrubberfollowedbyanexpandedbedbioreactorfortherecoveryofthespentcausticandforelementalsulfurgeneration.TheBiopuricprocessisalsoatwo-reactorsystem,whichcombinesaconventionalchemicalscrubberfollowedbyabiologicaltreatmentstep.Littleispubliclyknownaboutthelatterprocess.

Alternativeandsustainableprocessesneedtobedeveloped.Thus,thepurposeofthisstudywastoevaluatethetechnicalfeasibilityoftreatinghighconcentrationsofH2Sinlaboratory-simulatedbiogasorfuelgasusingasinglebiotricklingfilterreactor,andattempttoproducemostlyelementalsulfurwhichcanbeeasilydisposedorrecovered.Unliketheabovementionedcommercialsystems,thetreatmentdemonstratedinthispaperreliesonasinglereactorsystem.AlthoughH2Streatmenthadbeenwidelyreportedinbiofiltersandbiotricklingfilters(YangandAllen,1994;Devinnyetal.,1999;GabrielandDeshusses,2003a;KimandDeshusses,2005),thepresentstudyisdifferentbecauseitdealswithultra-highH2Sconcentrationsingasesthatareinitiallyoxygen-free.Operationatclose-to-neutralpHwaschoseninordertoimprovetheH2SabsorptioncapacityoftheliquidphasealthoughmanyoftheH2Sdegradingorganisms,likethegenusThiobacillus,haveacidicoptimumgrowingpH(RobertsonandKuenen,1999,2002).Also,absorptionandoxidationofH2StoelementalsulfurispHneutralasshownbyaddingEqs.

(1)and

(2).

Twolaboratory-scaleprototypeswithdifferentpackingmaterialswereusedtoevaluatetheperformanceintermsofH2Sremovalefficiency(RE=(Cin-Cout)/Cin)andeliminationcapacity(EC=(Cin-Cout)*Q/V,whereQisthegasflowandVisthebedvolume).TheratioofSO42-/S0producedunderdifferentoperatingconditionsaswellastherobustnessofthebioreactorwhenexposedtodifferentperturbationswerealsoassessed.

2.Materialsandmethods

BothexperimentalReactorsAandB(seeTable1)werebasedonthesamedesign(Fig.1)butwithslightlydifferentcharacteristics.Theyconsistedofabiotricklingfilterreactoroperatedinanupflow,counter-currentmode,fedwithamimicofbiogasorfuelgascontainingmostlynitrogen,CO2andH2Sasneeded.Althoughthegasdidnotcontainanymethaneorgaseoushydrocarbon,itwasareasonablemimicoffuelgasorbiogasforH2Streatmentpurposes.ThisisbecauseH2Sisdegradedbylithoautotrophicorganismswhichhavebeenshownnottobeaffectedbythepresenceoforganiccarbonsources(CoxandDeshusses,2002).Evenso,thepresenceofheterotrophicmethanotrophicbacteriawouldresultinsomecompetitionforoxygenwiththeH2Sdegraders.Sincemethaneisonlysparinglysolubleinwater(Sander,1999)andnotwelldegradedinbiofiltersorbiotricklingfilters(Nikiemaetal.,2005),onlyaslightamountofextraoxygenwouldneedtobesuppliedtocompensateforoxygenconsumptionbyheterotrophicorganisms.Duringtheexperiments,asmallmeteredstreamofair(asrequiredfortheaerobicoxidationofH2S)wasaddedtothebiogasorfuelgasmimic.

Mineralmediumcontaining(gl-1)KNO3,1;KH2PO4,1;K2HPO4,1;NaCl,1;MgSO4,0.2;CaCl2,0.02;traceelements(Pfenningetal.,1981),1mll-1forReactorAandNH4Cl,1;KH2PO4,1;K2HPO4,1;MgSO4.7H2O,0.5;CaCl2,0.25;traceelements(Pfenningetal.,1981),1ml1-1forReactorBwasalsocontinuouslyfedtosupplynutrientsandwashoutby-products.InorganiccarbonwassuppliedasCO2viathegasphase(ReactorA)ordissolvedHCO3-intheliquidphase(ReactorB).

ReactorAwaspackedwithrandomlydumped2*2*2cmcubesofopenporepolyurethane(PU)foam(EDT,Eckental,Germany).ThePUfoampackingwasdevelopedspecificallyforbiotricklingfiltration(GabrielandDeshusses,2003a;PhilipandDeshusses,2003;KimandDeshusses,2005).Ithasahighspecificsurfacearea(600m2m-3)andalowdensity(35kgm-3),arelativelyfinemesh(4–6porespercm),andalowcompressionstrength(5–10kPa).ThePUfoambedhadaninitialporosityofabout0.97.

ReactorBwaspackedwithpolypropyleneHDQ-PAC(LantecProductsInc.,CA,USA)witha4*4mmgridopening.TheHDQ-PACisacommonwetscrubberstructuredpackingwithaslightlylowerspecificarea(430m2m-3)thanthefoamandwiderpores.Acylinderofstructuredpackingwascuttotightlyfitinsidethebiotricklingfilterreactor.Theinitialbedporositywas0.88.HDQ-PACwasselectedbecauseofitsstructuralstrengthandbecauseitsopenstructuremayminimizetheretentionofsulfurexpectedfromtheproposedtreatment.

Reactorswereoperatedcontinuouslyforaperiodof3months(ReactorA)and7months(ReactorB)inordertotestarangeofoperatingconditions.Bothreactorswhereinoculatedwithsulfur-oxidizingbiomassinordertospeedupthestartupperiod.ReactorAwaspackedwithPUfoamcubestakenfromalab-scalebiotricklingfiltertreatinglessthan100ppmvH2S,whereasReactorBwaspackedwithcleanHDQ

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