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华中科技大学硕士学位论文二氧化碳矿化机制的实验研究姓名：徐俊申请学位级别：硕士专业：热能工程指导教师：张军营20060430I500K20158.05IIABSTRACTCoalisamainkindofenergysourceinChina,butcoalcombustionwillbringgreatpollutiontotheenviormentanddoharmtothehealthofhumanbeingsandlifeofwildplantsandanimalsinChina.Emissionandcontrolofcarbondioxide(CO2)fromcoalcombustionisnowanemergingandfrontierareaandgoingtoattractmoreattentioninfuture.Althoughthecarbondioxideseparationtechnicshavebeenfullmaturity,amassofcarbondioxideareemittedintoatmosphere.Carbonsequestrationasmineralcarbonatesisanovelmethodwithpotentialtobeimplementedwithacceptableeconomicstodisposecarbondioxideinlarge-scale.Someinnovativeresearchofcarbonsequestrationasmineralcarbonatesundermiddleandlow-pressurehasbeenmadeinthispaper.Inthefirstplace,thisarticlesummarizesthehazardsofcarbondioxidetotheenvironmentandsociety,thesourcesofcarbondioxideinatmosphereandthecurrentcontroltechnologiesintheworld.Explainthemineralcarbonationreactionmechanismintheoryaspect.Comparedtwodifferentmineralcarbonationreactionmodelsandanalyzedtheenergyequilibrium.Afterthat,thethermodynamicanalysishasbeencarriedoutusingtheMatlabprograms.Theresultsshowthatthemineralcarbonationreactioncanbeimplementedunderhigherpressurewhenthereactiontemperatureislowerthan500K.Thesolutionexperimentresearcheshavebeencarriedontheoscillatingthermostaticwater-bath.Theeffectofdifferentfactorswhichinfluencethesolutionoforeindistilledwatersuchastemperature,particlesize,thermaltreatmentandagitationhavebeenanalyzed.Ithasbeenobservedthatthehighestsolutionrateoforeindistilledwaterappearsduringthefirsttwentyminutes.Then,antigoriteorehasbeenchosentobetheoresampleformineralcarbonationexperimentduetothehigherdissolvability.Anexperimentplatformofcarbondioxidemineralcarbonationhasbeendesignedandbuiltaccordingtoparameterofthetest.Abundantexperimentalstudiesareperformedinthepapertoinvestigatethefactorsthatinfluencetherateofcarbonationreaction,suchasreactiontemperature,reactionpressure,particlesizeandpretreatment.X-raydiffractionIIIanalysis(XRD)identifiedmagnesiteastheprimaryreactionproduct,andunderoptimalconditions,58.05%stoichiometricconversionofthesilicatetocarbonatewasachievedin60minutes.Keywords:coalcombustioncarbondioxidesolutionmineralcarbonationcarbonsequestration2006430______“√”2006430200658111.11.1.12004[1]2030601.1[2]%%%%%%198572.820.92.04.3//200070.019.54.06.02.0/205060-705.05.06.010-205199412.427.7%20031620041920052170%1.1[2]201981690020044.473.9,520002.37220043.2520105.520207201065.5%1.22520.812.872SOx8793NOx6787CO285[3]SOxNOxCO2401.2SOx15.1CO213.2NOx10.1[4]1.1.2[5]441.5101.33kPa7831.17382kPa468kg/m356.6461kPa00.1kPa31.79Ncm3/g,1.0kPa15.92Ncm3/g31.0463.9kg/m3301074.2kg/m31/356,1/764.1“”1.1/3602100502.3.——4.5.4“”1.1.3ppm(V)1ppmV2.12GtC1Gt109t1GtC1Gt7.8GtCO21GtCO21GtCO2280ppmVCO2594Gt1991335ppmV752.6Gt25CO270%CO26085%CO21.2/51.2.1,,Fluor[6]CO2CO2H2130CO2Allied1965Selexol[7]CO2H2SCO2H2SH2SCO29H2SCO22050Rectisol[8]0CO21.2.2CO2CO2CO21.2.2.1CO2MEADEAADIPMDEACO26CO2[9]MEAMEA,CO2MEA,CO212%40%,30%80%,CO2,,,[10]CO2TEAMDEA{MEADEADETA}CO2[11]DETAMEADEADIPATEACO2DETAMDEAMEA56MDEADEAMDEAMEADEADIPAMEADEADIPA[12]TETACO2MEADEATEATETA1999CO2Gas/SpecCS22000,CO2,CO2Gas/SpecCS22000CO2[13]1.2.2.2[14]CO2CO2CO2CO21.2.2.3CO2CO223CO2702528CO27,15%CO285%N2CO2[15]:28%97%CO210%80%CO21.2.3CO2CO2CO21.2.3.1Ward[16]CO2/O2,HCO3-/CO32-CO2/O21500CO2/O24100LeBlanc[17],,,Teramoto[18,19]CO2,CO2,CO2CO2CO2(),,CO2,,Neplenbroek[20,21],,[22],,,,,Okabe[23]CO2,VAC(),K2CO38,,,1.2.3.2HFCLM,HFCLMGuha[24,25]HFCLM(CO2/CH4CO2/N2)20%,,N2H2HFCLM,HFCLM,(),,,[22,26]Papadopoulos[27],,,,CO2N2,,[25],,,,1.2.3.3,,980,,,,()(),[28-30]1),,2)/,,,3),(0),,,,4),,,,1.2.3.4EnvirogericsSystem[31]“Gasep”CO2,(10mm,12mm),,CO2,3Iwakami[32]CO2,CO2/CH420,CO26%1.7%;CO2/CH410,CO26%2.3%Okamoto[33].(PEO),Yoshikawa[34],CO2,,CO2/N2(6090),10,JintongLi[35]32(32methylsul-folane)CO2SO2PTMSMMACO2/N2(40),(2.5×10-8)Los-Alamos[36]polybenzimidazole(370)1.2.41234[37]1.31.3187272713630041191201:1.2.4.12050Whorton[38]CO2CO2CO2CO211WAGCO2Simon[39-40]CO2Bardon[41]CO2CO2Holm[42,43]CO2CO20.25-0.35/3CO2-Huang[44]122CO2Metcalfe[45]CO2CO2Orr[46]N2CO2CO2N2CO2N255CO2N2CO2CO2EORCO21.2.4.2CO2,,121.4131.4KCO2CH4N2304.15191.05126.15194.65109.1577.35Arri[47]CH4-CO2,,,Harpalani[48],LangmuirGreaves[49],[50]YukuoKatayama[51]Stevens[52],,[53],,,1.2.4.319931995AlbertaAlberta3[54]1996StatoilSleipnerWest141000mUtsira100×104t[55]IEA19961999SleipnerAquiferCO2Storage(SACS)[56][57]Texas2000“”1.2.51.51.5/,,[58]Robinson[59]:,15,2%(),,Sung[60]ChlorellaHA-1Menz[61],,,Kwata[62]:ShirainaYoshihiro[63]-CoA4TCA1.2.6CO2CO2Tester[64]1)CO2();2)CO2;3)CO21989,3.81300m86Nshikawa[65]CO2300bar275KOhgaki[66]NshikawaCO2CO2Shuichiro[67]CO25000mGolomb[68]CO21-20um16CO2CaCO2-CO2CaCO2CO2[69]CO2CO2CO21.2.7CO21.61.6Gf°(kcal/mole)CO2(g)-94.26HCO3-(aq)-140.31H2CO3(aq)-149.00MgCO3(s)-246.05CaCO3(s)-269.78Mg2SiO4(s)-490.28Mg3Si2O5(OH)4(s)-964.16Lackner[70]CO21.1CO2325422221/3()5/32/3HClMgSiOOHMgClHOSiO+→++(1-1)2422221/21/2HClMgSiOMgClHOSiO+→++(1-2)22()MgClHOMgOHClHCl+→+(1-3)222()()MgOHClMgOHMgCl→+(1-4)2223()MgOHC