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Studies On The Reaction Of Cyclohexene Epoxidation And Catalytic Properties Of Novel Titanium Silicalite-1

Posted on:2010-07-18Degree:MasterType:Thesis
Country:ChinaCandidate:X Y LiuFull Text:PDF
GTID:2181360275469313Subject:Organic Chemistry
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Since the titanosilicate molecular sieves TS-1 With ZSM-5 structure was reported,its outstanding selection of catalytic oxidation have been caused a great deal of concern.From the perspective of the research results to TS-1 for the oxidation catalyst used in the green oxidant hydrogen peroxide,with mild reaction conditions and high product selectivity,is expected to overcome a number of serious pollution of traditional crafts and harsh reaction conditions,which is developing a new type of environmentally friendly chemical process.China has listed TS-1 as a special catalytic material and successfully applied to the caprolactam production of new technology development which have independent intellectual property rights.A new type of catalytic oxidation materials - HTS-1 with novel hollow configuration was developed which is an international initiative.At the basis of previous studies,this thesis conducted more in-depth studies on the catalytic oxidation performance and acid catalytic properties of HTS-1.Cyclohexene catalyzed by HTS-1 was carried out with aqueous hydrogen peroxide as oxidant.The influences of various factors on the H2O2 utilization were investigated and the reaction conditions were optimized based on the previous studies.The impact of alkali additive on HTS-1 catalytic properties and catalyst regeneration method were also researched.The results showed that:HTS-1 in the catalytic hydrogen peroxide cyclohexene reaction process showed superior catalytic performance,Under the conditions of the V(acetone):V(cyclohexene) = 8,the mass concentration of the catalyst was 3%,n(H2O2):n (cyclohexene) = 1.7,T=55℃,t=8h,the conversion of cyclohexene could reach up to 89.11%and the selectivity of cyclohexene was 92.71%.The addition of appropriate amount of alkaline additive could not only improve the selectivity of epoxides,but also improve the catalytic activity of HTS- 1.In this paper,a preliminary exploration of cyclohexene epoxidation catalyzed by HTS-1 was carried out with self-made superoxide urea(UP) as oxidant in anhydrous environment.The results showed that HTS-1 in this system has good catalytic activity with UP as oxidant which can effectively avoid the occurrence of side reactions such as hydrolysis of epoxide compared to H2O2 as oxidant that significantly improved the cyclohexene selectivity and reduced the degree of difficulty in product analysis and separation.Except the comprehensive studies on the catalytic oxidation performance of HTS-1,this thesis also investigated the surface acid catalytic properties with hydrolysis reaction of 1,2 - cyclohexene oxide (EO) as a probe.The influences on the acid catalytic performence of TS-1 have been more in-depth studied and the qualitative and quantitative analysis of surface acidity of HTS-1 was carried out by the use of spectroscopy which provides a basis for reference to comprehensive understanding of catalytic properties of HTS- 1.
Keywords/Search Tags:HTS-1, cyclohexene, oxidation, acid property
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