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NH3-SCR performance and SO2 resistance comparison of CeO2 based catalysts with Fe/Mo additive surface decoration

氮氧化物 催化作用 氧化还原 初湿浸渍 化学 选择性催化还原 沉积(地质) 无机化学 硫酸盐 硫酸铵 反硝化 化学工程 氮气 选择性 有机化学 古生物学 工程类 燃烧 生物 沉积物
作者
Lin Zhu,Jie Yao,Gaofeng Ma,Ping Cao,Shiliang Wu,Zhaoying Li
出处
期刊:Chemical Engineering Journal [Elsevier BV]
卷期号:428: 131372-131372 被引量:71
标识
DOI:10.1016/j.cej.2021.131372
摘要

• The redox capacity of CeO 2 could be improved by in situ surface deposition of Fe 2 O 3 . • CeO 2 -Fe 2 O 3 showed the high NH 3 /NO oxidation ability and strong interaction with SO 2 . • CeO 2 -MoO 3 showed excellent SCR activity due to the enhanced surface acidity by MoO 3 . • Surface MoO 3 could inhibit catalyst sulfation and ammonium sulfate deposition. • The main SO 2 deactivation reasons were different for diverse CeO 2 based catalysts. Fe 2 O 3 and/or MoO 3 surface decorated CeO 2 were designed and synthesized by in situ deposition and incipient wetness impregnation to adjust the SCR catalytic performance and SO 2 resistance of CeO 2 . The addition of iron oxide slightly improved low temperature SCR activity of CeO 2 -Fe 2 O 3 , but resulted in a fast decline of NO x removal efficiency at higher temperatures, which was due to the enhanced NH 3 oxidation by surface redox capacity improvement. Surface acidity instead of redox capacity was the main limiting factor for SCR activity of CeO 2 and CeO 2 -Fe 2 O 3 . Meanwhile, the introduction of MoO 3 increased NO x conversion of CeO 2 -MoO 3 and CeO 2 -Fe 2 O 3 -MoO 3 dramatically in a broad temperature range. The increase of catalysts surface acid sites promoted their SCR catalytic performance through Eley-Rideal mechanism. SO 2 resistance test indicated the different surface characteristics for the four catalysts resulting from the composition disparity leaded to different deactivation behaviors at 250 °C. The deposition of ammonium sulfate species accounted for the main activity loss of CeO 2 and CeO 2 -Fe 2 O 3 , while the sulfation of redox sites was main deactivation reason for CeO 2 -MoO 3 and CeO 2 -Fe 2 O 3 -MoO 3 . The interaction between SO 2 and CeO 2 /CeO 2 -Fe 2 O 3 catalysts changed the surface active sites for SCR reaction essentially and MoO 3 could inhibited surface sulfation and ammonium sulfate species deposition. The variation behavior of NO x conversion during SO 2 resistance test depended on the reaction temperature. All four catalysts show the usability in the presence of SO 2 when the reaction temperature is between 300 °C and 400 °C. Considering the complexity of preparation process, catalytic performance and SO 2 durability, CeO 2 -MoO 3 catalyst is a better choice for substituting the traditional V-Ti catalyst.
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