摘要碳酸二甲酯(DMC)是一种对环境友好的绿色化学品，其洁净合成工艺的研究及开发，已引起国内外学者的广泛关注。以CuCl催化剂甲醇液相氧化羰化法合成DMC已实现工业化。由于反应生成了副产物HCl，造成Cl-的流失，不仅造成催化剂失活，同时对反应设备腐蚀严重，污染环境。论文中制备了CuCl和Schiff碱助剂络合均相催化剂，并采用IR对其进行了表征。考察了不同Schiff碱助剂（助剂：CuCl=1：1）对CuCl催化甲醇液相氧化羰化合成DMC催化性能的影响。结果表明：N-甲基咪唑与CuCl络合制备的催化剂催化活性最高。在120℃，反应压力2.4MPa，反应时间4h条件下，甲醇的转化率达到5.8%，DMC的选择性达到99.9%。对于双配体络合CuCl催化体系，能进一步提高催化活性。在120℃，反应压力2.4MPa，反应时间4h，聚乙烯吡咯烷酮：N-甲基咪唑：CuCl=2：1：1(摩尔比)，甲醇的转化率达到6.6%。结果同时表明，催化体系的Cl-的流失量降低，催化剂的寿命得到了提高。关键词：氧化羰化甲醇；碳酸二甲酯；铜络合物催化剂AbstractDiethylcarbonate(DMC)isanenvironmentallybenignintermediation.ItwaspaidwidelyattentionthattheresearchanddevelopmentofagreenprocessofsynthesisofDMC.AlthoughtheprocessofproducingDMCbyoxidativecarbonizationofmethanolinthepresenceofCuClcatalystsystemhasbeenindustrial,somedrawbacks,forinstancetheproductionoftheby-productionHCl,inwhichnotonlycausedtoaleakingofCl-subsequencebythedeactivateofthecatalyst,butalsoacorrosiontothereactor,stillneedtobeovercome.Inthiswork,acomplexcatalystwaspreparedfromCuClandSchiffbaseadditivesandcharacterizedbyIR.TheeffectsofdifferentSchiffbaseadditiveswereinvestigated.TheresultsshowedthathighactivitywasexhibitedinthepresenceofcomplexcatalystsynthesizedbyN-methylimidazoleandCuCl，themethanolconversionwas5.8%,DMCselectivityreachedto99.9%at120,pressure2.4MPa,thereactiontime4h.Atthesamecondition,catalytic℃activitywasfurtherimprovedbytwo-ligandscomplexCuClsystem,methanolconversionis6.56%(PVP:N-methylimidazole:CuCl=2:1:1).TheresultalsoshowedthatlifeoftheCuCl/Schiffbaseadditivecatalystswasprolonged.Keywords:oxidativecarbonizationofmethanol；DMC；Cuprouschloridecomplexcatalys目录摘要..........................................................................................................................................IAbstract...........................................................................................................................................II第一章文献综述.........................................................................................................................11.1碳酸二甲酯的性质..............................................................................................................................11.1.1物理性质..................................................................................................................................11.1.2化学性质.....................................................................................................................................11.1.3碳酸二甲酯的应用..................................................................................................................11.2碳酸二甲酯的合成工艺......................................................................................................................21.3国内外的研究状况................................................................................................................................21.4甲醇液相氧化羰化合成碳酸二甲酯的热力学计算......................................................
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