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Study of the catalytic combustion of lean hydrogen-air mixtures in a monolith reactor

机译:整体反应器中贫氢空气混合物的催化燃烧研究

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This paper presents an experimental study of catalytic hydrogen combustion that used commercial catalysts containing Pt in a honeycomb monolith reactor in a plug flow configuration. The emphasis is on determining global kinetics in the case of low hydrogen content. Measurements of the temperature and composition of the reaction product at the outlet in the steady state condition at the different initial compositions of hydrogen and total volumetric feed rates were performed. The conversion of hydrogen was determined in parallel to the composition of the reaction product at the outlet using GC as well as by means of the thermodynamic approach using material and energy balances. The influence of the flow rate and initial molar fraction of hydrogen on hydrogen conversion is shown. A kinetic expression of the Arrhenius type is proposed with the reaction first order in hydrogen and zero order in oxygen for the overall process of the oxidation of hydrogen in lean hydrogen-air mixtures. The determined activation energy was in good agreement with the desorption activation energy for O-2 from graphene-covered Pt(111) surfaces using temperature-programmed desorption. This result shows transport-limitations for heterogeneous hydrogen conversion in catalytic hydrogen combustion. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
机译:本文介绍了催化氢气燃烧的实验研究,该燃烧氢气在活塞整体结构的蜂窝状整体反应器中使用了含Pt的商用催化剂。重点是在氢含量低的情况下确定整体动力学。在不同的氢气初始组成和总体积进料速率下,在稳态条件下,对出口处反应产物的温度和组成进行了测量。氢气的转化率与出口处反应产物的组成平行,使用GC以及通过使用材料和能量平衡的热力学方法确定。显示了氢气的流速和初始摩尔分数对氢气转化率的影响。提出了Arrhenius类型的动力学表达式,其中氢在稀氢-空气混合物中氧化的整个过程中,氢反应为一级,氧反应为零级。所确定的活化能与使用程序升温脱附的石墨烯覆盖的Pt(111)表面中O-2的脱附活化能高度吻合。该结果显示了催化氢燃烧中非均相氢转化的传输限制。 (C)2018氢能出版物有限公司。由Elsevier Ltd.出版。保留所有权利。

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