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Study On Ni-Based Catalysts For Methane, Carbon Dioxide And Oxygen Catalytic Oxidation And Reformation To Synthesis Gas

Posted on:2002-08-13Degree:DoctorType:Dissertation
Country:ChinaCandidate:T JiFull Text:PDF
GTID:1101360185474186Subject:Industrial Catalysis
Abstract/Summary:PDF Full Text Request
It is one of promising ways that producing synthesis gas from nature gas. Steam reformation of methane has been industrialized for many years, but it has too many shortcomings, then study of partial oxidation of methane and carbon dioxide reformation of methane have became new focus throughout the world. Partial oxidation of methane to synthesis gas is an exothermic reaction and carbon dioxide reforming methane to synthesis gas is an endothermic reaction. Combining both reactions leading to thermal coupling can tone CO/H2 ratio of products and inhibit carbon deposition, which are very important in nature gas industry. Based on correlative references, catalytic oxidation and reformation of methane, carbon dioxide, and oxygen to synthesis gas by Ni-based catalysts was studied in this paper. According to nature of this reaction system, a design process of catalysts was taken out. Catalysts were evaluated by a fix bed reactor to screen one with best performance. An investigation of operating conditions was made as well. Catalysts were characterized by many modern analysis techniques, such as XPS, XRD, TPR, TG, and SEM, to obtain the relationships of activity, components and structure. Carbon deposition on catalyst surface was studied deeply as well.The optimum catalyst was obtained after performance evaluation. Catalyst 12%Ni-5%Ce-3%Mn-2%Li/γ-Al2O3(wt.) have excellent activity and stability. The better preparation method is layer immersion (additives immersing first), calcining at 773K and 1123K for 2 hours and 8 hours respectively, particle size is 20-40 mesh. The better operating conditions of reaction by using Ni-Ce-Mn-Li/γ-Al2O3 catalyst as follow:After reducing catalysts with 50ml/minN2+30ml/minH2 at 1073K for 3 hours, the reaction system can get to thermal equilibrium with different feed stocks ratio, yield of CO and H2 more than 93% and 95% respectively, and CO/H2 ratio can be adjusted easily between 05-1.0 without activity decrease. The lifetime of catalyst is more than 120 hours.
Keywords/Search Tags:methane, synthesis gas, Ni-based catalyst, carbon deposition, reaction mechanism
PDF Full Text Request
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