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Kinetics of methane combustion over Pt and Pt-Pd catalysts

机译:甲烷燃烧动力学/ Pt和Pt-Pd催化剂

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摘要

A kinetic study was performed over thermally aged and steam-aged Pt and Pt-Pd catalysts to investigate the effect of temperature, and methane and water concentrations on the performance of catalysts in the range of interest for environmental applications. It was found that both catalysts permanently lose a large portion of their initial activity as result of exposure to 5 vol.% water in the reactor feed. Empirical power-law and LHHW type of rate equations were proposed for methane combustion over Pt and Pt-Pd catalysts respectively. Optimization was used to determine the parameters of the proposed rate equations using the experimental results. The overall reaction orders of one and zero in methane and water concentration was found for stabilized steam-aged Pt catalyst in the presence and absence of water. The apparent self-inhibition effect caused by methane over Pt-Pd catalyst in the absence of water was associated with the inhibiting effect of water produced during the combustion of methane. A significant reversible inhibition effect was also observed over steam-aged Pt-Pd catalyst when 5 vol.% water vapor was added to the reactor feed stream. A significant reduction in both activity and activation energy was observed above temperatures of approximately 550 C for steam-aged Pt-Pd catalyst in the presence of water (the activation energy dropped from a value of 72.6 kJ/mol to 35.7 kJ/mol when temperature exceeded 550 °C).
机译:在热老化动力学研究steam-aged Pt和Pt-Pd催化剂研究温度的影响,和甲烷和水的浓度催化剂的性能范围的利益环境的应用程序。两种催化剂永久失去很大一部分他们的最初活动接触的结果5 vol. %的水反应堆饲料。幂律和LHHW类型的速率方程提出了在Pt和Pt-Pd甲烷燃烧催化剂分别。确定的参数提出率方程使用实验结果。订单1和0的整体反应甲烷和水浓度被发现稳定steam-aged Pt催化剂的存在和无水。self-inhibition效应引起的甲烷没有水是Pt-Pd催化剂与水的抑制效应燃烧过程中产生的甲烷。重要的也是可逆的抑制效果5时观察到在steam-aged Pt-Pd催化剂vol. %水蒸气添加到反应堆饲料流。观察和活化能温度大约550度steam-aged Pt-Pd催化剂的存在水从一个值(活化能下降72.6焦每摩尔35.7焦每摩尔,温度超过550°C)。

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