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The Research Of Catalystic Synthesis Of Pyrrole And Pyrrole N-substituents

Posted on:2015-03-04Degree:MasterType:Thesis
Country:ChinaCandidate:Z Q PanFull Text:PDF
GTID:2181330431492199Subject:Chemical processes
Abstract/Summary:PDF Full Text Request
Cu/ZnO, Cu/ZnO/Al2O3, Cu/ZnO/ZrO2, Cu/ZrO2and Cu/Ni/ZrO2synthesized byco-precipitation method for ethanol dehydrogenation amination reaction was effective tocatalyze the formation of C-N. In this paper,1,4-butanediol as feedstock as feedstock reactedwith Ammonia or methylamine to synthesize pyrrole and N-substituted pyrrole, respectively.These catalysts were charactered by XRD、TPR、NH3-TPD and N2O decomposition to furtheranalysize the catalytic mechanism.The research that Cu/ZnO, Cu/ZnO/Al2O3, Cu/ZnO/ZrO2, Cu/ZrO2, Cu/Ni/ZrO2wereapplied to1,4-butanediol dehydrogenation amination reaction for pyrrole showed Cu/ZnO,Cu/Ni/ZrO2had a good catalytic activity, and further studied. As for Cu/ZnO catalyst, Cu0was the reactive species and ZnO as catalyst carrier well played a role in the dispersion of Cuspecies to increase Cu0surface area and finally improve the catalytic performance of thecatalyst. Based on the research about the catalytic performance of the catalyst with a differentCu/Zn mole ratio, the catalytic performance was best when the Cu/Zn mole ratio was1:1. Asfor Cu/Ni/ZrO02catalyst, Cuand Cu3.8Ni were the reactive species ZrO2as catalyst carrier forproviding a certain number of acid sites to promote the synthesis of pyrrole. By studying thedifferent preparation conditions of the co-precipitation method, Cu/Ni/ZrO2catalyst reflectedthe excellent catalytic performance when the pH of titration endpoint was7.5~8.5, theprecursor solution aged for4h at70℃and the precursor was calcinated for12h at500℃. Byinvestigating the parameter of1,4-butanediol dehydrogenation amination reaction forpyrrole, the selectivity for pyrrole was better at the condition that airspeed was0.44h-1, thereaction temperature was280℃and the molar ratio of alcohol and ammonia was1:1.UsingCu/Ni/ZrO2as catalyst and Methylamine as ammonia source, the studies showedmethylamine as ammonia source in place of ammonia successfully synthesized N-methylpyrrole.However, acetamide as ammonia source did not synthesize the expected N-acetylpyrrole.
Keywords/Search Tags:Cu catalysts, Cu/ZnO, Cu/Ni/ZrO2, pyrrole, pyrrole N-substituents
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