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Study On Pd-based Catalyst Over Anthraquinone Hydrogenation Reaction

Posted on:2014-05-30Degree:MasterType:Thesis
Country:ChinaCandidate:Y C GuanFull Text:PDF
GTID:2181330422468325Subject:Chemical Engineering
Abstract/Summary:PDF Full Text Request
Hydrogen peroxide (H2O2) is an important chemical reagent which has beenwidely used in the industrial fields of electronic, pharmaceutical, papermaking,hairdressing, desinfection and so on. In the commercial production, hydrogenperoxide is produced by the process of2-Elthylanthraqunion (2-EAQ) hydrogenationand oxidation (AHO). In the whole AHO process, hydrogenation reaction of2-EAQ isthe key process because it was related to the economic benefit of the whole process.Therefore, Pd based catalyst with high catalytic activity and selectivity for thehydrogenation reaction is required.In this dissertation, the effects of the factors during Pd/γ-Al2O3preparationprocess on its catalytic performance were investigated, and the bimetallic Pd-Aucatalyst which loaded by different order was also investigated. Firstly,Pd/γ-Al2O3catalyst was prepared by impregnation method, and the effects of supportpartical size and pore size, the calcination temperature of the support, theimpregnation temperature and calcination temperature of the catalyst were studied forthe hydrogenation reaction. The results indicated that smaller partical size and largerpore size of the support was in favour of the reaction, and suitable calcinationtemperature and dipping temperature could improve the interaction between metal andsupport. Based on those results, the effect of loading order of Pd and Au on thehydrogenation activity of bimetailic Pd-Au catalyst was investigated. The resultdemonstrated that added Au could improve the hydrogenation efficency of Pd-basedcatalyst for the2-EAQ hydrogenation reaction greatly.The promotion mechanism of additives Au for anthraquinone hydrogenationreaction was revealed by different experimental characterization (BET, XRD, H2-TPR,CO-TPD, TEM and XPS) and density functional theory. The results indicated that theaddition of Au could improve the geometric and electronic properties of Pd-basedcatalyst. The added Au got electrons from Pd, which was in favour of the existence ofthe low valence state Pd which had high catalytic activity. What’s more, addition Aucould enhance the activation of carbonyl bond in2-EAQ. Therefore, thehydrogenation efficiency of2-EAQ to produce H2O2is eventually promoted.
Keywords/Search Tags:Pd/γ-Al2O3catalyst, bimetallic Pd-Au, anthraquinonehydrogenation deaction, density functional theory
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