Fe-ZSM-5分子筛上N_2c2_O一步氧化苯制苯酚工艺条件与本征动力学分析

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1、ABSTRACToPERAT玎呵GCONDITIONGSANDINTR"叮SICl(INETICSOFoNE．STEPOXIDATIONOFBENZENEToPHENOLWITHNITROUSoXIDEOVERFe．ZSM．5CATALYSTABSTRACTBasedontheexperimentsinanisothermalintegralreactor(中21X3mm，L450mm)，theeffectsoftemperature(350～500。C)，spacevelocity(2500-10000h‘1)andbenzene／nitrousm

2、olarratio(2～12)onbenzenetophenolwithnitrousoxideoverFe—ZSM-5zeolitecatalyst(includingselectivity,conversionandproductyield)wereinvestigatedbythesingle-factortestmethodunderawideexperimentalrange，respectively．Theresultsshowed：(1)Withtheincreaseoftemperature，theconversionofN20inc

3、reasedandtheselectivityofphenoldecreased，theproductivityandyieldofphenolfirstincreasedandthendecreased．(2)Withtheincreaseofspacevelocity,theconversionofN20decreasedandtheselectivityofphenolincreased．Appropriatespacevelocitywasbeneficialtoimprovetheproductivityofphen01．(3)Withth

4、eincreaseofbenzene／nitrousmolarratio，theconversionofN20andtheselectivityofphenolincreased．Buthi曲benzene／nitrousmolarratiowouldresultinthedecreaseofphenolproductivity．ⅡI北京化工大学硕士学位论文Theglobalinfluenceoftemperature，spacevelocityandbenzene／nitrousmolarratioontheoxidationreactionand

5、productdistributionwasalsoinvestigatedbymeansoftheorthogonaltestofL16(45)．Theoptimalconditionsweredeterminedasfollows：temperature400。C，spacevelocity6000h一，benzene／nitrousmolarratioof5：1．UsingthemessagewhichfromdistributionofproductsbasedontheGC-MS，andbasedonthethermodynamicanal

6、ysis，themainreactionandmainsidereactionweredeterminedandthereactionnetworkforoxidationofbenzenetophenolwithnitrousoxidewasproposed，whichcanreasonablyexplaintheexperimentalphenomenainthiswork．TheintrinsickineticexperimentsofoxidationofbenzenetophenolwithnitrousoxideFe-·ZSM--5zeo

7、litecatalystwerecarriedoutinanintegralmicro-reactor(①6×2mm，L300mm)underthefollowingconditions：temperatureof380*C-450*C，benzene／nitrousmolarratioof8-12andspacevelocityhigherthan12000h～，PowerLawtyperateequationsofthissystemwereestablishedonthebasisofreactionnetworkproposedhere．Th

8、eparametersofthekineticmodelswereestimatedbymeansofSim