LaY沸石中La离子定位的研究

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:2006207217:973(G2000048001):,Tel:010282368646;E2mail:panhh@ripp2sinopec.com:100128719(2007)0320087205LaYLaSTUDYONLANTHANUMCATIONLOCATIONINLaYZEOLITE,,,,PANHui2hua,HEMing2yuan,SONGJia2qing,TIANHui2ping,ZHUYu2xia(,100083)(ResearchInstituteofPetroleumProcessing,SINOPEC,Beijing100083,China):2LaY,XRDRietveldLaY,LaS,O3,,2LaYLaO3LaYLaO3,LaO32LaY,La3O3,2,La[La(OH)2]+2,Na+SLaY,Al,Al3+S:LaY;;;;:TE624.9:AAbstract:LaYsampleswerepreparedbydoubleexchangedoublecalcinations(DEDC)methodandliquid2solidphaseexchange(LSPE)method.Theposition,occupationandcoordinationofLa3+outsidetheframeworkofYzeoliteweredeterminedbypolycrystallineXRDwiththeRietveldmethod.La3+situateatSsitesandcoordinatewithframeworkoxygen(O3).Asaresult,theymadetheframeworkofYzeolitemorestableandthehydrothermalstabilityimproved.InsamplespreparedbyLSPEmethod,theinteractionbetweenLa3+andO3wasstrongerbecausethebonddistancefromLa3+toO3wasshorterthanthatinsamplespreparedbyDEDCmethod.InsamplespreparedbyLSPEmethod,Lacationexistedintheformof[La(OH)2]+becauseeachLa3+coordinatedwithtwohydroxylbesidesthreeO3.TherewereasmallamountofNa+locatedatSsitesinsidehexagonalprisminsamplespreparedbybothmethods.InsamplespreparedbyDEDCmethod,therewereafewAl3+locateatSsitesduetoslightdealuminationduringpreparationprocess.Keywords:LaYzeolite;lanthanum;rareearth;Rietveldrefinement;rareearthcationsite,REYREHY[1-8]Y,SO3,Al,Y;B,[9]REYREHY,,,()20076ACTAPETROLEISINICA(PETROLEUMPROCESSINGSECTION)233©1994-2008ChinaAcademicJournalElectronicPublishingHouse.Allrightsreserved.(RIPP)2,XRDRietveld2LaYLa11.1NaY,88%,Na2O13.6%,2.468nm,Na56Al56Si136O384NaYLaCl37H2O(,)2LNY2LLNY2SL(a0)(CR)(SZ)11LNY2LLNY2SLTable1Physico2chemicalpropertiesofLNY2LandLNY2SLsamplesSamplea0/nmCR/%SZ/(m2g-1)w(La2O3)/%w(Na2O)/%UnitcellcompositionLNY2L2.46847.160617.21.8H1.6Na8.1La15.1Al56Si136O38432.8H2OLNY2SL2.47049.662017.21.6H3.1Na7.3La15.2Al56Si136O38434.5H2O1.2D5005XCuK,,40kV,40mA,,0.02,2s,570MicromeriticsASAP2405NV1.011.3310-2Pa3004h,N2,77.4K,t2plot(SZ)1.3XLaY,D/max2500,CuK,K1=0.15406nm,K2=0.15443nm,I(K2)/I(K1)=0.5;40kV,150mA;,0.02DS=1,SS=1,RS=0.15mm,5s,88522.1LNY2LLNY2SL1LNY2LLNY2SLXRDNH+4,I311/I222[10]LNY2SLI311/I2223.9,LNY2LI311/I2221.2,LNY2SLLNY2L1LNY2LLNY2SLXRDFig.1XRDpatternsofLNY2LandLNY2SLsamples(1)LNY2L;(2)LNY2SL2.2,hkl,,Rietveld[11]Rietveld,,,88()23©1994-2008ChinaAcademicJournalElectronicPublishingHouse.Allrightsreserved.[12]NaY[13](,Fd3m(No227))TO1O2O3O4:,,,T(Si,Al);0.5(96/192),Fourier,Rietveld,PseudoVoigt(PV),(4350)(LNY2L39,LNY2SL36),Rietveld2RpRwp,2,10%15%2LNY2LLNY2SL342LNY2LLNY2SLRietveldTable2ResultsofRietveldrefinementforLNY2LandLNY2SLSamplea0/nmRp1)Rwp2)23)LNY2L2.46640950.0780.1551.18LNY2SL2.47020160.0810.1631.261)Rp=0Io,i-Ic,i0/Io,i,Io,iandIc,iaretheobservedandcalculatedpowderdiffractionintensitiesfortheithpointrespectively;2)Rwp={[wi(Io,i-Ic,i)2]/[wi(Io,i)2]}1/2,wi=1/Io,i;3)2=(Rwp/Re)2,Re=[(N-P)wi(Io,i)2]1/2,NisthenumberobservedpowderdiffractiondatapointsandPisthenumberofrefinedparameters.FAU,192,1,LNY2LLNY2SL5,,2LNY2LLNY2SLXFig.2TheobservedandcalculatedXRDpatternsandtheirdifferencediagramforLNY2LandLNY2SLsamples(a)LNY2L;(b)LNY2SL(1)Io;(2)Ic;(3)Bragg2position;(4)Io-IcIoObservedXRDintensity;IcCalculatedXRDintensity,LNY2L1.8Na+,11.8LaS,1.5LaLa,La2LNY2SL1.4Na+,14LaS,1.8La,28.6La,La,[La(OH)2]+983LaYLa©1994-2008ChinaAcademicJournalElectronicPublishingHouse.Allrightsreserved.(O2-0.132nm,La3+0.106nm),LaO3,LNY2SLLaO3LNY2L,LNY2SLLaO3LaO2,La3+O2LNY2SLLaOH0.2666nm,3O3,LaLNY2LAl3+O2O3,0.3

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