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Support acidity effects of NiMo sulfide catalysts in hydrodenitrogenation of quinoline, indole and Coker Gas Oil

Abstract : The thesis objective is to identify the support acidity effects of sulfide catalysts in hydrodenitrogenation (HDN) reactions in order to improve the HDN catalysts.Kinetic data obtained from quinoline and indole HDN, over NiMo(P)/Al2O3 and NiMo(P)/ASA catalysts were analyzed by a Langmuir-Hinshelwood kinetic model, including liquid-vapor mass transfer, in order to estimate kinetic and adsorption parameters. Kinetic modeling results indicated that the NiMo(P)/ASA catalyst favored the hydrogenation of 1,2,3,4-tetrahydroquinoline into decahydroquinoline, which is the rate limiting step of quinoline HDN. However, the promoting effect of the NiMo(P)/ASA in hydrogenation steps of indole HDN was not evidenced. In quinoline and indole HDN, the NiMo(P)/ASA showed a strong promoting effect in N-removal reactions. Nitrogen compounds adsorb more strongly over NiMo(P)/ASA. Characterization by Infra-Red spectroscopy of CO suggested that these results might be related to the modification of the electronic properties of promoted NiMoS phase due to higher acidity of ASA.The HDN of quinoline-indole mixture showed a strong inhibiting effect of quinoline on indole HDN whereas the inhibiting effect of indole on quinoline HDN was negligible over NiMo(P)/Al2O3 and more important over NiMo(P)/ASA. The HDN of a mixture of Straight Run and Coker Gas Oil allowed an access to the HDN mechanism and comparison of reactivity towards HDN of different compounds. The HDN of neutral compounds was inhibited by the stronger adsorption of basic compounds. Carbazole-type and quinoline-type compounds were refractory. The NiMo(P)/ASA likely favored more cracking reactions and as well showed a faster deactivation rate than the Al2O3 counter catalyst
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Minh Tuan Nguyen. Support acidity effects of NiMo sulfide catalysts in hydrodenitrogenation of quinoline, indole and Coker Gas Oil. Chemical engineering. Université de Lyon, 2016. English. ⟨NNT : 2016LYSE1209⟩. ⟨tel-01673792⟩



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