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Reaction Kinetics of the Hydroenitrogenation of Decahydroquinoline over NiMo(P)/Al_2O_3 Catalysts

机译:NiMo(P)/ Al_2O_3催化剂上十氢喹啉加氢氮化的反应动力学

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The reaction mechanism and the kinetics of hydrodenitrogenation (HDN) of decahydroquinoline (DHQ) over NiMo(P)/Al_2O_3 catalysts were studied in the presence and absence of H_2S. Cis- and trans-propylcyclohexylamine were identified as the most important reaction intermediates; thei reactivity was found to vary under different reaction conditions. The kinetic constants in the HDN network of DHQ were calculated assuming a Langmuir-Hinshelwood mechanism. It was found that, in the phosphorus-containing catalysts, the adsorption of DHQ was enhanced and the rate constant of the first C-N bond cleavage decreased. As a consequence, the overall HDN reaction rate of DHQ decreased when phosphorus was added to a NiMo/Al_2O_3 catalyst. The effect of H_2S was the opposite of that of phosphorus: it increased the rate constants and decreased the adsorption constants. The inhibiting effect of DHQ in its own conversion was different from that on the hydrogenation of cyclohexene, proving that different catalytic sites are involved in these reactions.
机译:研究了在存在和不存在H_2S的条件下,十氢喹啉(DHQ)在NiMo(P)/ Al_2O_3催化剂上的反应机理和动力学。顺-和反-丙基环己胺被认为是最重要的反应中间体。发现反应性在不同反应条件下变化。假设Langmuir-Hinshelwood机制,计算DHQ的HDN网络中的动力学常数。发现,在含磷催化剂中,DHQ的吸附增强,并且第一次C-N键裂解的速率常数降低。结果,当将磷添加到NiMo / Al_2O_3催化剂中时,DHQ的总体HDN反应速率降低。 H_2S的作用与磷相反:它增加了速率常数,降低了吸附常数。 DHQ在其自身转化中的抑制作用不同于对环己烯氢化的抑制作用,证明这些反应涉及不同的催化位点。

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