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Activating low-temperature NH3-SCR catalyst by breaking the strong interface between acid and redox sites: A case of model Ce2(SO4)3-CeO2 study
Journal of Catalysis ( IF 6.5 ) Pub Date : 2021-05-11 , DOI: 10.1016/j.jcat.2021.05.001
Jiawei Ji , Meizan Jing , Xiuwen Wang , Wei Tan , Kai Guo , Lulu Li , Xin Wang , Wang Song , Lijun Cheng , Jingfang Sun , Weiyu Song , Changjin Tang , Jian Liu , Lin Dong

The occurrence of NH3-SCR (selective catalytic reduction of NO with NH3) reaction on catalyst surface typically requires acid and redox sites. However, the role of acid-redox interaction on NH3-SCR performance is still obscure due to complex acidities and entangled acid-redox sites. Herein, three types of model Ce2(SO4)3-CeO2 catalysts with distinct interfaces are constructed to reveal the effect of acid-redox interaction on NH3-SCR performance. That is, SO42-/CeO2-VS (vapor sulfation of ceria) with strong acid-redox interfacial contact, SO42-/CeO2-WI (wet impregnation), and SO42-/CeO2-SG (solid grinding) with limited interfaces. It is found the redox property is significantly disturbed as a result of the electron-withdrawing effect from the sulfate. Theoretical result unravels that the introduction of Ce2(SO4)3 retards the oxygen vacancy formation over CeO2. Due to restricted interfaces in SO42-/CeO2-SG, the negative influence from acid sites is greatly alleviated. Further mechanism study discloses the weakened acid-redox interaction actually changes the nature of surface NOx species, resulting in the generation of reactive species (*O-N-O* and cis-N2O22-) and the promotion of surface reaction via Langmuir-Hinshelwood (L-H) mechanism.



中文翻译:

通过破坏酸性和氧化还原位点之间的强界面来激活低温 NH 3 -SCR 催化剂:以 Ce 2 (SO 4 ) 3 -CeO 2 模型研究为例

在催化剂表面发生 NH 3 -SCR(NO 与 NH 3 的选择性催化还原)反应通常需要酸和氧化还原位点。然而,由于酸度复杂和酸-氧化还原位点缠结,酸-氧化还原相互作用对NH 3 -SCR 性能的作用仍不清楚。在此,构建了三种具有不同界面的模型Ce 2 (SO 4 ) 3 -CeO 2催化剂,以揭示酸-氧化还原相互作用对NH 3 -SCR性能的影响。即,SO 4 2- /CeO 2 -VS(二氧化铈蒸气硫酸化)与强酸-氧化还原界面接触,SO 42- /CeO 2 -WI(湿法浸渍)和 SO 4 2- /CeO 2 -SG(固体研磨)界面有限。发现由于硫酸盐的吸电子效应,氧化还原性能受到显着干扰。理论结果表明,Ce 2 (SO 4 ) 3的引入延缓了CeO 2 上氧空位的形成。由于 SO 4 2- /CeO 2 -SG 中的界面受限,酸性位点的负面影响大大减轻。进一步的机制研究揭示减弱的酸-氧化还原相互作用实际上改变了表面 NO x的性质物种,导致产生活性物种(*ONO*和顺式-N 2 O 2 2-)并通过 Langmuir-Hinshelwood (LH) 机制促进表面反应。

更新日期:2021-06-01
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