催化作用
拉曼光谱
空位缺陷
原位
氧气
氧化还原
吸附
材料科学
化学工程
无机化学
化学
结晶学
物理化学
有机化学
工程类
光学
物理
作者
Lei Chen,Dan Ren,Xiaoke Hou,Jinping Zhang,Yang‐wen Wu,Yibio Wang,Chao Hu,Peigao Duan,Chao Li,Ching‐Yu Chiang,Chi He,Qiang Lü
标识
DOI:10.1016/j.apcatb.2023.123202
摘要
The development of highly active and SO2-resistant catalysts is a major hurdle in the catalytic oxidation of NO to NO2. Herein, we fabricate a core–shell Mn2O3 @CeO2 catalyst using a two-step method for NO oxidation. Benefiting from the generation of abundant Mn4+−Ov−Ce3+ interfacial sites and plentiful oxygen vacancies, the resulting Mn2O3 @CeO2 exhibits a superior low-temperature NO-to-NO2 capacity (T50 at 183 °C and T86 at 275 °C), obtaining a remarkable temperature reduction compared to commercial Pt/γ-Al2O3 catalyst (T50 at 262 °C). Meanwhile, In-situ Raman and In-situ Drifts reveal that Mn4+−Ov−Ce3+ interfacial site is the main adsorption site for the formation of N-containing intermediates, which plays a decisive role in the NO oxidation reaction. More encouragingly, SO2 shows a much higher affinity for CeO2 sheath (ECeO2,SO2= –3.48 eV) than Mn2O3 core (EMn2O3,SO2= –0.87 eV), thus avoiding its toxic effects on the interior active sites and endowing Mn2O3 @CeO2 a superior SO2-resistance.
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