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Modulating multi-active sites in CeO2-modified MnOx/ZSM-5 catalyst for selective catalytic oxidation of diethylamine
Applied Catalysis A: General ( IF 4.7 ) Pub Date : 2022-10-30 , DOI: 10.1016/j.apcata.2022.118929
Lin-Cong He , Xu-Fang Wang , Chu-Feng Liu , Bei Li , Meng-Fei Luo , Jian Chen

An efficient MnOx/CeO2/ZSM-5 catalyst was developed for selective oxidation of diethylamine (DEA) with high N2 selectivity in a wide temperature window (ΔT = 140 °C), owing to the existence of oxidation and selective catalytic reduction (SCR) active sites. MnOx species prefer to locate on the surface of CeO2 compared to ZSM-5, and the presence of CeO2 is beneficial to form more Mn4+ species, the active sites for oxidation reaction. The mechanistic investigation suggests that internal SCR of NOx generated from the over-oxidized DEA is the crucial pathway for N2 generation. The high SCR activity of the MnOx/CeO2/ZSM-5 catalyst in oxidation conditions is mainly attributed to the synergistic catalysis of Mn4+ species and acid sites of ZSM-5, the active sites for SCR reaction. Thus, it has been clearly clarified that addition of CeO2 and its addition sequence could modulate the surface active sites of MnOx/ZSM-5 catalyst for the selective catalytic oxidation of DEA.



中文翻译:

调节 CeO2 修饰的 MnOx/ZSM-5 催化剂中的多活性位点用于二乙胺的选择性催化氧化

由于存在氧化和选择性催化作用,开发了一种高效的 MnO x /CeO 2 /ZSM-5 催化剂,用于在宽温度窗口(ΔT = 140 °C)内具有高 N 2 选择性乙胺(DEA)选择性氧化还原(SCR)活性位点。与ZSM-5相比,MnO x物种更倾向于位于CeO 2的表面,并且CeO 2的存在有利于形成更多的Mn 4+物种,即氧化反应的活性位点。机理研究表明,由过氧化的 DEA 产生的 NO x的内部 SCR 是 N 2的关键途径。一代。MnO x /CeO 2 /ZSM-5 催化剂在氧化条件下的高 SCR 活性主要归功于 Mn 4+物种和 SCR 反应活性位点 ZSM-5 的酸性位点的协同催化作用。因此,已经清楚地阐明了CeO 2的添加及其添加顺序可以调节MnO x /ZSM-5 催化剂的表面活性位点,用于DEA的选择性催化氧化。

更新日期:2022-11-01
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