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Preparation And Catalysis Performance Of CeO2-catalyst For 1, 4-Butanediol Selectivity Dehydration

Posted on:2012-11-17Degree:MasterType:Thesis
Country:ChinaCandidate:C ChenFull Text:PDF
GTID:2211330368989667Subject:Physical chemistry
Abstract/Summary:PDF Full Text Request
3-buten-1-o1 contains two kinds of functional group, double bonds and hydroxide radical. It can be used in the oxidation, reduction, esterification and addition reaction, etc. It is an important medicine intermediate and can be widely used in synthsis of new medicine for heterocyclic derivative, which showed satisfactory efficacy in treating AIDS, arthritis and chronic pneumonia. The traditional method for synthesis of 3-buten-l-ol by propylene-formaldehyde addition or by 3,4-epoxy-l-butylene reduction, both of them have many disadvantages such as high temperature, high pressure or low yield. Synthesis of 3-buten-1-ol by dehydration of 1,4-butanediol is a novel way,The study of high activity catalyst is still a key problem.The synthesis of 3-buten-1-ol by dehydration of 1,4-butanediol via CeO2 catalysis has been reported. But the investigated CeO2 catalyst was primarily commercial reagent. The preparation chemicals of CeO2 for the reaction had not studied. In this paper, The CeO2 catalysts were prepared by hydrothermal precipitation with Ce(NO3)3-6H2O as precursor and Na3PO4 as mineralize. The effect of different preparation conditions on structure and catalytic performance of CeO2 catalyst have been studied. The paper further studied the properties of Zr-CeO2, Ca-ZrO2 catalysts. The main results and conclusions are as follows:1. CeO2 catalyst prepared by hydrothermal precipitation showed better catalysis performance for the synthsis of 3-buten-1-o1. The prepare condition of CeO2 catalyst by hydrothemal precipitation was investigated. Meanwhile, the properties and structure of catalyst was charactered by XRD, BET, TEM, TPR etc. CeO2 catalyst showed great catalytic activity on the condition of hydrothermal temperature is 200℃, the viscosity of mineralize is 0.003mol/L, sintering temperature is 450℃.(1)Different prepared condition were used to prepare the CeO2 catalysts and resulted in different morphologies. The catalysts prepared by hydro- thermal temperature 200℃, the concentration of mineralize 0.003mol/L, sintering temperature 450℃. The CeO2 sample was acquired with regular rectangle morphology, well-grown crystalline and preferentially exposed (111) facets, which showed excellent activity and selectivity for synthesis of 3-buten-1-ol by the selective dehydration of 1,4-butanediol, and the conversion of 1,4-butanediol was 95.8%, with 3-buten-1-ol yield of 60.7%.(2)With the calcined temperatue increasing, the catalysts sinters, and the activity decreases.2. The effect of different metal oxide catalysts and compound oxide catalysts on the synthesis of 3-buten-l-ol was investigated. It was found that ZrO-CeO2 and CaO-ZrO2 catalyst formed solid solution. The doped cerium oxide showed excellent anti-sinter ability, which had better catalysis ability in the synthesis of 3-buten-1-ol by dehydration of 1,4-butanediol.
Keywords/Search Tags:CeO2, 1,4-butanediol, 3-buten-1-ol, selective dehydration
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