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The Research Of Catalysts, Comonomers And Reactions For CO2Copolymerization

Posted on:2014-03-22Degree:MasterType:Thesis
Country:ChinaCandidate:T W HuFull Text:PDF
GTID:2251330401973144Subject:Chemical processes
Abstract/Summary:PDF Full Text Request
Since the mid-20th century, the amount of industrial carbon dioxide emissions increased dramatically, which caused the global warming, climate anomalies, ecological imbalance and a series of serious consequences. The same time, CO2is a renewable carbon resource, and is abundant in nature, non-toxic, non-flammable, inexpensive and easy to get. It is of great significance to achieve the CO2copolymerization with epoxy compound, the reaction can produce the degradable polycarbonate material, which is conducive to the recovery and utilization of CO2, environmental protection, easing the oil resources crisis.In this thesis, the catalysts, monomers and reactions of CO2copolymerization were researched. The contents and the main conclusions are as follows:1. Salicylaldehyde ethylenediamine Salen-metal catalysts were prepared, and these homogeneous catalysts were loaded on the molecular sieve to synthesize heterogeneous catalysts using the microwave and impregnation method. The chiral3,5-di-tert-acetyl salicylic aldehyde cyclohexyl diamine Salen-metal catalyst were also synthesized. The Characterizations of IR, UV, and TGA showed that the target homogeneous and heterogeneous Salen-metal catalysts were obtained.2. Poly (o-aminophenol) is synthesized by a facile chemical polymerization without any surfactants or templates. Sphere-like microstructures of PoAP are obtained via self-assembling of two dimensional nanoplates, and the possible formation mechanism of PoAP microstructures follows the prickly-fluffy-full sphere growth process. By susceptibility test, PoAP synthesized in this study exhibite superior and sustained antibacterial effect against the typical gram-positive B. subtilis. In addition, morphologies of the obtained PoAP microstructures show obvious influences on its antimicrobial efficacy, the looser the microspheres structure is, the better their antibacterial activity would be.3. The POAP loaded with Metal salts or Salen-metal catalyst can be used as homogeneous catalysts in reaction, but heterogeneous separation after reaction by changing the solvent. The Characterizations of IR, UV, TGA and XPS showed that the target catalysts were obtained. These catalysts possess good thermal stability, and they can be applied to most of the reaction. However, metals and Salen-metal catalyst loading amount are low.4. Salicylaldehyde ethylenediamine Salen-metal and the supported catalysted a-pinene epoxidation reaction to prepared a-epoxypinane, and the optimum reaction conditions were obtained by single factor method and response surface methodology: the reaction temperature is0℃, the reaction time was6h, the amount of catalyst is6mg. Under this optimum reaction conditions, a-epoxypinane yield is74%, the result is close to the predicted valueof response surface methodology. Compare to the homogeneous salen-metal catalyst, the catalytic activity heterogeneous catalyst is not a serious decline, the a-epoxypinane yield could reach50%or more. And after five recycle, its catalytic yield of the reaction is not significantly decreased.5. The POAP/Salen-metal catalysts could successfully catalyze the CHO/CO2copolymerization. Using IR, G and MS to characterize the polymerization product, the results show that, cobalt metal and chrome metal catalytic of POAP/salen were effective for the CHO/CO2reaction, but the catalytic activity of POAP/SalenCrCl2is higher, its highest conversion rate up to78.73%, the selectivity of the polycarbonate was51.36%, the yield of the polycarbonate up to1.98g.6. Under different reaction conditions, The POAP/Salen-metal catalysts were used to catalyze the a-epoxypinane/CO2copolymerization. IR, GC and MS were employed to characterize the reaction mixture, unfortunately, the CO2polymerization reaction does not occur, nor cyclic carbonate generated.
Keywords/Search Tags:CO2, Poly (o-aminophenol), Salen-metal catalysts, α-epoxypinane, Copolymerization
PDF Full Text Request
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