取代甲撑肼基二硫代甲酸酯热裂解和羰基化合物催化硅氢加成新型催化剂研究-有机化学专业论文.docxVIP

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取代甲撑肼基二硫代甲酸酯热裂解和羰基化合物催化硅氢加成新型催化剂研究-有机化学专业论文.docx

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取代甲撑肼基二硫代甲酸酯热裂解和羰基化合物催化硅氢加成新型催化剂研究-有机化学专业论文

AbstractThegas-phasepyrolyticreactionsofmethylsubstituted-methylidenehydrazinedithio- carboxylate and the novelcatalystofhydrosilylation ofketone were studied.Thetechniqueofpyrolyticreactionisbasedonthethermaldecompositionofthematerial duringthethermaltreatments.Anumberoforganicmoleculescouldbedecomposedtoother moleculeswhenheated.Thegas-phasepyrolyticreactionsofmethylsubstituted- methylidenehydrazinedithiocarboxylatewerestudiedbyGC/MSfirstly.Theresultsshowedthat methyl3-aryl-methylidenehydrazinedithiocarboxylatecouldbecleavagedtoaromaticcyanate, methylthiolandHNCSintheinletoftheGC/MSinstrument.Therelationshipofthermal decompositionwiththebasetemperatureoftheinletwasstudied,findingthatthetemperaturewas an important key to the gas-phase pyrolytic reaction. The series of these compounds weredecomposedcompletelyatthebasetemperatureof230℃.Meanwhilethepyrolyticcleavageofdifferentsubstitutesat210 ℃wasalso studied.The results showed thatthe compoundssubstituted withelectrondonating groupscouldbecleavagedmuch morecompletelythantheonessubstitutedwith electron withdrawing groups atthe same temperature.Apossiblemechanismforthegas-phasepyrolyticreactionwasproposed.Thegas-phase eliminationofthemono-substitutedcompoundsispostulatedthatitunderwentasix-membered ringtransitionstateandafour-memberedringtransitionstates.Thegas-phaseeliminationofthe di-substitutedcompoundscanonlyproceedafour-memberedringtransitionstateproducing isothiocyanate becauseofthe absenceofthe γ-Hofthe compounds.Secondaryalcoholsareofgreatsignificanceoftheseintermediatesforthemanufactureof pharmaceuticalsandadvancedmaterials.Thecatalytichydrosilylationasdirectroutetosecondary alcoholsisamongthemostattractive.Oneofthemajoradvantageofthisprocessliesinthe extremelymildconditionsrequiredand technicalsimplicity,ascomparedtootherreduction methods such ashydrogenation.Aneweffectiveapproachofthesynthesisofsecondaryalcoholhasbeendeveloped.With ZnX2ascatalyst,hydrosilylationofalargevarietyofketonesisreportedforthefirstti