石墨衍生物固体酸催化果糖脱水制备5-羟甲基糠醛的分析-analysis of preparation of 5 - hydroxymethylfurfural by solid acid catalyzed dehydration of fructose with graphite derivatives.docxVIP

AbstractInrecentyears,theincreasingdepletionoffossilfuelscausestheseriousenergycrisisandenvironrnentalpollutionwhichisbringingharmtothepeople’slives.Thus,developingtherenewablebiomassresourcesbecomesmoreandmoreimportantnow.Researchshowsthatchemicalconversionofbiomassfeedstockisausefulmethodtoproducethehighvalue-addedpharmaceuticalintermediatesandmonomerofpolymerfromsustainableresources.Therein,thecatalyticdehydrationof6-Csugarbiomasscangenerate5-hydroxymethylfurfural(5-HMF),andthentoprepareusefulcompoundssuchaspharmaceuticalproducts,fuelandpolymerthroughthehydrogenation,oxidation,halogenation,hydrolysis,esterificationandaldolcondensationreaction.Inthisthesis,thedehydrationofhexosesto5-HMFcatalyzedbygraphite-derivedsolidacidcatalystshasbeenstudied.Thepreparationofthehighcatalyticactivityandstabilityofmetal-freesolidcatalystsaremainlyinvestigasted,andtheircatalyticperformancesonthedehydrationreactionarestudiedindetail.Firstly,thesolidacidcatalystgraphiteoxide(GO)waspreparedwithamodifiedHummers’method,andthenisfurtheremployedtothecatalyticdehydrationoffructose.Asaresult,itwasfoundthattheoptimumamountofcatalystGOis0.1g,theoptimumreactiontemperatureis120℃,theoptimumreactiontimeis3.5hours,theoptimumreactionsolventisdimethylsulfoxide.Undertheoptimalconditions,theyieldof5-HMFarrivesat60.6%.Moreover,GOwasfurthertreatedbyhightemperatureandstrongbase/acid,whicharerespectivelydenotedash-GOandn-GO,theircatalyticperformancesaresimliarwiththatofGOinthedehydration,andtheyieldof5-HMFis63.0%or61.8%,respectively.Ontheotherhand,thedehydrationofinulincatalyzedbythegraphiteoxideGOwasalsostudied.Theoptimalreactiontemperatureis160℃,theoptimumreactiontimeis4.0hoursandtheoptimumreactionsolventisH2O:THF(V:V)=1:3;Itwasfoundthata61.2%yieldof5-HMFisobtainedunderthesuitableconditions.Secondly,thecompositepolyaniline-graphiteoxide(PANI-GO)ispreparedfrominsitupolymerizationofanilineinthecolloidalGOsolution.Futhermore,thesulfatedPANI-GO2-(SO4/PANI-GO)isalsopreparedviathesulfationprocessusinga70%conc