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Sulfur poisoning and regeneration of Rh-ZSM-5 catalysts for total oxidation of methane
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-05-28 , DOI: 10.1016/j.apcatb.2020.119176
Yu Zhang , Peter Glarborg , Martin Peter Andersson , Keld Johansen , Thomas Klint Torp , Anker Degn Jensen , Jakob Munkholt Christensen

The activity of Rh/ZSM-5 catalysts for methane oxidation was investigated under conditions simulating the exhaust from lean burning, natural gas fueled engines to evaluate the influence of reaction atmosphere on catalytic activity. The Rh-catalysts yield high methane conversion at conditions achievable in real exhaust systems, despite the inhibiting effects of H2O and SO2. The influence of temperature and SO2 concentration (1−20 ppm) on the activity were studied. The deactivation caused by SO2 was intensified with decreasing temperature and increasing SO2 concentration, and the SO2-poisoning could be modeled as the occupation of active sites following a Temkin adsorption isotherm. At 400 °C essentially full coverage of S-species was reached with 1−2 ppm of SO2, but at 500 °C the coverage had decreased significantly, and considerable catalytic activity was preserved in the presence of SO2. Significant activity was regenerated in SO2-free gas, but the nature of the SO2-free regeneration atmosphere was unimportant.



中文翻译:

Rh-ZSM-5催化剂的硫中毒和再生,可完全氧化甲烷

在模拟稀燃天然气燃料发动机的废气条件下,研究了Rh / ZSM-5催化剂的甲烷氧化活性,以评估反应气氛对催化活性的影响。尽管有H 2 O和SO 2的抑制作用,但Rh催化剂在实际排气系统中可达到的条件下仍能产生较高的甲烷转化率。研究了温度和SO 2浓度(1-20 ppm)对活性的影响。引起的SO减活2是随着温度的降低和增加加剧SO 2浓度,和SO 2毒化可以建模为Temkin吸附等温线后活动位点的占用。在400°C下,1-2 ppm的SO 2基本上达到了S物种的完全覆盖,但是在500°C下,该物种的覆盖率显着降低,并且在存在SO 2的情况下保留了相当大的催化活性。在不含SO 2的气体中再生了显着的活性,但是不含SO 2的再生气氛的性质并不重要。

更新日期:2020-06-23
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