|Thesis Advisor||侯震山 ; 吾满江·艾力|
|Place of Conferral||北京|
|Keyword||二氧化碳 环氧化合物 环碳酸酯|
Carbon dioxide is the industrial waste product and the main components of the greenhouse gases. Research studies to convert CO2 into many useful products to reduce the carbon dioxide emission are increased over the past decades. Coupling of CO2 and epoxides to synthesis cyclic carbonates is one of the most promising methodologies in this area. Cyclic carbonates can be used as excellent aprotic polar solvents, precursors for producing polycarbonates, fine chemicals, and etc. From the study of activation of carbon dioxide and the Process and mechanism of the formation of cyclic carbonates via epoxides and carbon dioxide catalyzed by the catalysts were detailed documented. (1) The first section described that the low cost KI/MCM-41 catalyst could be easily prepared by the incipient wetness impregnation of MCM-41 with aqueous solution of KI. Several techniques were employed to confirm that KI was well-dispersed onto the surface of MCM-41. The formation of propylene carbonate was used as a test reaction for the activity of catalysts. The present study demonstrates that KI/MCM-41 (KI, 35 wt %) catalyst has given excellent catalytic activity to produce cyclic carbonates from CO2 and epoxides. In the consideration of the experimental results and previous reports, the mechanism of the cycloaddition of cyclic carbonates from epoxides and CO2 catalyzed by supported KI/MCM-41 catalyst was proposed. (2) The second section described a novel and mild method for the synthesis of cyclic carbonate using the KI/PER system free of solvent. The cheapness, easy availability of the reagents, short reaction time, and excellent yield of the products are the advantages that make this protocol a useful addition to the existing methodologies. (3) In third section, a convenient and simple way is presented to immobilize adenine onto zirconium phosphonates. This series of catalyst were prepared for the synthesis of cyclic carbonates from epoxides and carbon dioxide. Their porous and layered structure and surface morphology were characterized by nitrogen adsorption-desorption, XRD, SEM and TEM. The influence of the linkage lengths on the catalytic performance was also investigated. Typical optimized catalyst 1c, with a larger pore diameter, was found to be more catalytic active than the other catalysts. Moreover, the catalyst 1c was easily separated from the reaction systems and could be reused for several times without significant loss of catalytic activity. (4) Zirconium phosphonates-supported bromide quaternary ammonium salts are reported in the fourth section for the first time as recyclable and efficient catalysts for the synthesis of propylene carbonate from propylene oxide and carbon dioxide, which requires no additional organic solvents either for the reaction. This catalyst 1d also has given excellent catalytic activity in the synthesis of various carbonates. The catalyst 1d was easily recovered and could be reused at six times without much loss of activity. In addition, the reaction mechanism was discussed on the basis of the experimental results. (5) In fifth section, a series of zirconium phosphonates-supported 1-butylimidazole catalysts 1a-e could be easily prepared. Several techniques were employed to confirm that the low cost 1-butylimidazole was successfully grafted onto the zirconium phosphonates-supports. The formation of propylene carbonate was used as a test reaction for the activity of catalysts. The present study demonstrates that heterogeneous catalyst 1d has given excellent catalytic activity to produce cyclic carbonates from CO2 and epoxides. Furthermore, it could maintain high catalytic performance and stability without much loss in catalytic activity, even in the fifth reused time. In the consideration of the experimental results and previous reports, the mechanism of the cycloaddition of cyclic carbonates from epoxides and CO2 catalyzed by zirconium phosphonates-supported 1-butylimidazole catalysts was proposed.
|周亮. 催化二氧化碳与环氧化合物制取环碳酸酯的研究[D]. 北京. 中国科学院大学,2014.|
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