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Study of sulfur poisoning on Pd/Al2O3 and Pd/CeO2/Al2O3 methane combustion catalysts

机译:Pd / Al2O3和Pd / CeO2 / Al2O3甲烷燃烧催化剂中硫中毒的研究

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In the present work the CH4 combustion behavior of Pd/Al2O3 and Pd/CeO2/Al2O3 catalysts in the presence of SO2 is investigated under various reaction conditions. Attention is paid also to the behavior of the bare supports without the active phase. Both fresh and poisoned samples are characterized by IR spectroscopy and in situ CO adsorption. Transient activity measurements after SO2 poisoning indicate that regardless of CeO2 loading a strong deactivation of all catalysts is observed compared to fresh samples. The effect of sulfur poisoning on steady state activity at 653 and 873 K is also measured. The deactivation is evident only at 653 K and its dynamics reflects the dynamics of SO2 adsorption. Results of TPD experiments under inert or reaction atmosphere suggest that the dynamics of SO2 desorption is influenced by the combustion reaction taking place on the catalyst active sites. Ceria-doped catalysts are more sensitive to the composition of the atmosphere of adsorption/desorption and quantitative measurements indicate that the presence of CeO2 inhibits SO2 adsorption under reaction conditions.
机译:在目前的工作中,在各种反应条件下研究了Pd / Al2O3和Pd / CeO2 / Al2O3催化剂在SO2存在下的CH4燃烧行为。还应注意没有活动阶段的裸支撑的行为。新鲜样品和中毒样品均通过红外光谱和原位CO吸附进行表征。 SO2中毒后的瞬态活性测量表明,与新鲜样品相比,无论CeO2负载如何,都观察到所有催化剂的强烈失活。还测量了硫中毒对653和873 K时稳态活动的影响。失活仅在653 K时才明显,其动力学反映了SO2吸附的动力学。在惰性或反应气氛下进行的TPD实验结果表明,SO2解吸的动力学受到催化剂活性位点上发生的燃烧反应的影响。掺杂二氧化铈的催化剂对吸附/解吸气氛的组成更敏感,定量测量表明,在反应条件下,CeO2的存在抑制了SO2的吸附。

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