Asymmetric oxygen vacancy-enriched Mn2O3@CeO2 for NO oxidation with excellent low-temperature activity and boosted SO2-resistance

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 plent...

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Veröffentlicht in:Applied catalysis. B, Environmental Environmental, 2024-01, Vol.340, p.123202, Article 123202
Hauptverfasser: Chen, Lei, Ren, Dan, Hou, Xiaoke, Zhang, Jinping, Wu, Yangwen, Wang, Yibio, Hu, Chao, Duan, Peigao, Li, Chao, Chiang, Ching-Yu, He, Chi, Lu, Qiang
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Sprache:eng
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Zusammenfassung: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. [Display omitted] •A two-step hydrothermal approach was adopted to fabricate Mn2O3@CeO2 for NO oxidation.•Abundant Mn4+−Ov−Ce3+ sites form at manganese−cerium interfacial perimeter.•Mn4+−Ov−Ce3+ interfacial sites of Mn2O3@CeO2 boost the low-temperature activity.•The CeO2 sheath improves SO2-resistant ability of Mn2O3@CeO2.
ISSN:0926-3373
1873-3883
DOI:10.1016/j.apcatb.2023.123202