改性β沸石催化环己酮肟气相Beckmann重排反应的研究

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1、、÷毒!蚩兰”‘少⑧天津大蓦中目近代第一M太学博士学位论文一级学科：丝主王捏与撞盔学科专业：丝茎王苎作者姓名：童越i指导教师：王亚拯塾撞天津大学研究生院ABSTRACT￡-Caprolactamisavaluablestartingmaterialforthemanufactureofnylon6andresins．Beckmannrearrangementofcyclohexanoneoximetoe-caprolactamisoneofthemostimportantprocessesintheproductionofe-caprolactam．Thecurren

2、tlyusedtechnologyfortheBeckmatmrearrangement,catalyzedbyliquidacids，suffersseveraldrawbacks：antieorrosiveequipmentbeingrequiredandtheproductionoflargeamountsoflowvaluebyproducts．So，itisofgreatimportancetofindlowpollution,moreactiveandmorestabilitysolidacidcatalysts，whichcanrenderthereac

3、tiontobeoperatedinthevaporphase．Inthepresentwork,zeolitepwasfirstsynthesizedbyahydrothermalmethod；B203／Hp，M003／HBcatalystswe∞preparedbyimpregnationmethod；Hpwastreatedbyalkaline；H—nBWaSpreparedbyisomorphoussubstitutionofAIin13zeolitebyTi．AllthecatalystsobtainedwerecharacterizedbyXRD，BET,

4、IR．XPSandTPDete．，andstudiedinthevaporphaseBeckmannrearrangementofcyclohexanoneoxime．Also．H-ZSM-5zeolitewimdifferentratiosofSi02／A1203andthemesoporousH·Si—MCM-41werecomparedwitllHpinthisreaction．FortheHp—supportedB203catalysts，thesupportedB203with<20．33wt．％loadingsmainlyincreasedtheamoun

5、toftheweakBronstedacidsitesandshowedbettercatalyticstability,whiletheloadingsofB203>20．33wt．％coveredtheacidsitesanddecreasedthecatalyticstability．Loading3．66wt．％M003onHBalsomainlyincreasedtheamountoftheweakBronstedacidsitesandshowedbettercatalyticstability．However,witllloadingsof16．46wt

6、．％M003ledtothestructuralbreakageofzeoliteptosomeextent．TheframeworkTiintheHpzeoliteincreasedtheamountofweakBronstedacidsitesandimprovedthecatalytiestability,whiletheamorphousTi02favoredthesidereactions．Thecatalyststreatedinammonia，ethanolamine，orethylenediaminesolutionsshowedbettercatal

7、yticstabilityduetotheformationofmoreweakBronstedacidsims．111eresultsrevealedthattheactivesitesforthevaporphaseBeckmannrearrangementofcyclohexanoneoximewerenotidenticalondifferentcatalysts．Onzeolite13-basedcatalysts，theactivesitesmightbetheweakBroustedacidsites．Onthecatalystshav