從甲烷經(jīng)非合成氣過程制備醋酸的新流程.pdf

1、湖南大學碩士學位論文從甲烷經(jīng)非合成氣過程制備醋酸的新流程姓名：王寬新申請學位級別：碩士專業(yè)：化學工藝指導教師：周小平20050501==壘量鎏黧i!窒堡堇薹羹羹l叁墼墼墼塹鎏羹!AbstractMethaneisthemajorcomponentofnaturalgas，andalsoarichnatureresourcettishighlydesiredtodevelopenergysavingprocessestoconvertme

2、thanetooxygenates，suchasaceticacidAceticacidisanimportantfeedstockinchemicalindustry，whichissynthesizedbymethanolcarbonylationandmethanolisobtainedfromnaturalgasorcoalviasyngasprocessThisprocessneedsahighenergyinputMoret

3、hanonefourthofnaturalgasorcoalmustbeburnedtogenerateheatforthesteamreformationofnaturalgas(above800“C)orcoal(above12004C)Meanwhile，largeamountofgreenhousegasisformed，andthemethanolsynthesisreaction(fromH2andco)isahighpre

4、ssure(above50atm)reactionInthisworkwedesignedanonsyngasprocessforaceticacidsynthesisTheprocessconstitutesthat，methanewasprimarilyreactedwithHBrandoxygentoproduceCH3BrandCOoveraRu／Si02catalyst，andthen，theas—producedCH3Bra

5、ndCOwasconvertedtoCH3COBroveraRhCl3一PPh3catalyst，whichwasfinallyhcdrotyzedtoaceticacidandHBrInourprocess，methanewasconvertedtobromomethane，COandH20byreactingmethane，oxygen，andHBr／H20Morethan69％ofmethaneconversionwasreach

6、edinasinglepass，withCH3BrandCOasmajorcarboncontainingproductsandCH2Br2asbyproductOurstudyalsoindicatedthatamixtureofbromomethaneandCOwithamoleratiocloseto1：1couldbeachievedbyadjustingreactionconditionsor／andusingdifferen

7、tcatalystsTheaceticacidsynthesisreactionveascarriedoutinapressurizedbatchreactorWaterandcatalystwerepreloadedintothereactor，andwhichwasthencooleddownto504CandliquidCH)BrwasloadedintoitunderthetemperatureThereactorwaspres

8、surizedto26armwithCO◇990％)ineveryrun，andthenheatedtodesiredreactiontemperatureforcertainperiodofreactiontimeItmakeslargedifferenceswhetherthewaterisaddedbeforethereactionWhenwaterwasaddedinthecarbonylationreaction，therea

9、ctionwasveryslowWhenwithoutwater。thecarbonylationofCH3Brproceededatamuchtasterrate。Inthisresearchwork，wehaveinvestigatedtheinfluenceofcatalyst，cocatalyst，temperature，pressure，reactiontime，andsolventonreactionrateTheresul