n,2o一步氧化苯制苯酚的催化剂研制与性能分析

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1、北京化工大学硕士学位论文N<,2>O一步氧化苯制苯酚的催化剂研制与性能分析姓名：张宪国申请学位级别：硕士专业：化学工艺指导教师：李建伟20060504摘要利。相对而言，选择800℃的焙烧预处理温度比较适宜。利用xRD、NI-13。TPD、”A1MASNMR、FTIR、XPS、UV-vis葺tlH2．TPR等方法对Fe-ZSM-5分子筛高温焙烧前后的性能变化进行了表征，结果表明：(t)Fe离子以非骨架铁的形式负载于Fe-ZSM一5分子筛的表面或孔道中，其存在态为Fe203；(2)高温焙烧处理导致分子筛发生骨架脱铝，并在表面形成新的五配位铝；(3)高温焙烧使Fe-ZSM-5

2、表面的Fe203含量降低，所诱发的Fe离子表面迁移形成了更多有利于苯酚生成的活性位，因而能显著提高苯酚的选择性。关键词：分子筛，苯，N20，苯酚，金属离子改性，高温焙烧Ⅱ摘要PreparationandPerformanceAnalysisontheCatalystsofOne-stepOxidationofBenzenetoPhenolwithNitrousOxideABSTRACTAseriesofcatalystsforone—stepoxidationofbenzenetophenolwithnitrousoxidewerepreparedbymeansofio

3、n—exchangedmethodsandbythiswaythezeolitesofdifferentstructures(p，MCM-22，ZSM-5)weremodifiedwithmetalions(Fe3+，Cu2+，K+，Pd2+，Ce3+，La3+)．ThesamplesofcatalystswerepretreatmentwithhightemperaturecalcinationunderN2ambience．Bysinglefacturexperimentmethod，theeffectofprocessconditions，suchastemper

4、ature，spacevelocity,molarratioofbenzenetoN20etcwasexperimentallyinvestigatedinanisothermalintegralreactor．Basedontheexperimentalresults，theperformanceevaluationconditionsofthecatalystswgredefined：atmosphericpressure，400"t2，afeedconcentrationof50m01％benzene，5m01％N20，and45m01％helium，spacev

5、elocity4636h1．Theeffectsofthemolarratioofsilicontoaluminium，Fe-ioncontent，metalions，zeolitestructure，hi曲temperaturecalcinationpretreatmentonthecatalystperformancewereinvestigatedbasedontheevaluationconditionsmentionedaboveandthepreparedcatalystspowder．Theresultsshowed：(1)Withtheincreaseo

6、fthemolarratioofsilicontoaluminium．theconversionoflII摘要N20decreasedandtheselectivityofN20tophenolincreased．(2)WiththeincreaseofFe—ioncontent，theconversionofN20increasedandtheselectivityofN20tophenoldecreased．(3)Theperformanceofiron—exchangedZSM-5zeoliteswasbetterthantheoneofcopper-exchan

7、gedZSM一5zeolites．ThemetalionsK，Pd2+，Ce3+，La3+)hadlittleeffectonimprovementofzeoliteslifetime．(4)TheperformanceofFe—ZSM-5zeolitewithMFIstructurewasobviouslymoreadvantageousthantheoneofFe-MCM-22zeolitewithMWWstructureandtheoneofFe—BzeolitewithBEAstructure．(5)Thehightemperat