CO偶聯(lián)制草酸酯工藝條件及催化劑失活與再生研究.pdf

1、天津大學(xué)碩士學(xué)位論文CO偶聯(lián)制草酸酯工藝條件及催化劑失活與再生研究姓名：項(xiàng)鐵麗申請(qǐng)學(xué)位級(jí)別：碩士專業(yè)：化學(xué)工藝指導(dǎo)教師：李振花20031201AbstractTllesynthesisofdialkyloxalatebycatalyticcouplingreactionofcarbonmonoxidewasanenvironmentallybentgnandatomiceconomyreactionprocessAnewmethodwa

2、sadoptedt0prepareethylnitritewithconcentrationover95％Thesynthesisconditionsofdiall(yloxalatebyCOcouphgwereinvestigatedTberesultsshowedthattheoptimumresideneetimedecreasedwiththeincreaseoftheconcentrationofethylnitritandt

3、hedecompositiondegreeofethylnitriteincreasedToachieveahigheryieldofdiethyloxalatetheconcentrationofethylni扛iteshouldbelessthat20％and也ereactiontemperatureat393卅03KThedecompositionreactionofethylnitritewascarriedoutandther

4、esultsshowedthatthedecompositiondegreeincreasedwiththeincreaseofreactiontemperaturetherest出licetimeandconcentrationofethylnitriteThisindicatedthatthedecompositionreactionofethylnitritecompetedwithC0couplingreactionSothet

5、hreeconditionsshouldbelimitedincertainrangeOnthesamePd／FecatalystthesynthesisofdimethyloxalatebymethylnitritewascomlmredwiththesynthesisofdiethyloxalateanditwasfoundthatthesDacetimeyieldofdimethyloxalateiShigherthandieth

6、yloxalateonthesameconditionsThereasonmaybethatthedecompositiondegreeofmethylnitriteiSlowerthanethylnitriteThisresultwasofgreatimportancetoestablishtheoptimalconditionofCOcouplingreaction11蟛supporteffectwasstudiedanditwas

7、foundthatPdFe／a—Aj201wasbetterthanPdFe忙A120stosynthesizediethylo)【alateinbothreactivityandstabilityThespecificsurfaceareaandporestructuredistributionwereimportantfactorforsametypeofsupport11站reactiontemperatureofCOcoupli

8、ngreactiontodiethyloxalatewasartificiallyrunawaytocertaintemperature，whichcausedthecatalyticdeactivationThenthecatalystswereregeneratedandthentheactivitywasmeasuredagainDeactivatedcatalystswerefurtheranalysedby)①SThedeac

9、tivationvcasmainlyduetosinteringathightemperatureandoxidationofpdotopd2whentemperaturewasrunawayto673K～773KandthecatalyticactivityoftheregeneratedcatalystscouldhefollyrecoveredWhenthetemperaturewasruna、vayto1273K～1473K，t

10、hedeactivationwasduetocovetingofactivePdbvotherelementsandthecatalyticactivityofregeneratedcatalystscouldberecoveredpartiallyThisprovidedthewayteusethedeactivatedcatalystsKeywords：coupling，carbonmonoxide，support，diethylo