Experimental study of Fe modified Mn/CeO2 catalyst for simultaneous removal of NO and toluene at low temperature
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摘要: 本研究采用浸渍法制备了Fe改性的Mn/CeO2催化剂，并测试了催化剂在低温条件下同时脱硝与脱甲苯的性能。结果表明，Fe5Mn/CeO2催化剂表现出最佳的催化性能，甲苯的转化效率在175 ℃达到90%，NO转化率在95–300 ℃达到90%。通过BET、SEM、XRD、XPS、H2-TPR、NH3-TPD和O2-TPD等表征手段对催化剂的理化性质进行分析。XPS结果表明，Fe5Mn/CeO2催化剂中Ce3 + 和Mn4 + 的含量增加，促进氧空位和不饱和化学键的形成，提供了更多的活性位点，从而有利于在低温下高效脱除NO和甲苯。H2-TPR、NH3-TPD和O2-TPD表征表明，与其他催化剂相比，Fe5Mn/CeO2催化剂具有优异的氧化还原能力、更强的酸性和更好的氧迁移能力。此外，本研究还探究了Fe5Mn/CeO2催化剂上选择性催化还原（NH3-SCR）反应与甲苯催化氧化反应之间的影响。其中，NH3优先吸附活性位点而抑制了甲苯吸附，而NO2的生成促进了甲苯催化氧化反应；甲苯对NH3-SCR反应的抑制作用随着温度的升高而减弱，在100 ℃时，甲苯对NH3-SCR反应的抑制作用消失。超过225 ℃后，甲苯作为还原剂与NO发生反应且促进了NO2的生成，从而对NH3-SCR反应有促进作用。Abstract: A series of Mn/CeO2 catalysts modified with different Fe contents were prepared by impregnation method and tested for their low-temperature performance for simultaneous de-nitrification and toluene removal. It was found that the Fe5Mn/CeO2 catalyst showed the best catalytic performance and the conversion efficiency of toluene reached 90% at 175 ℃ and NO conversion reached 90% at 95−300 ℃. The physical and chemical properties of the catalysts were characterized by BET, SEM, XRD, XPS, H2-TPR, NH3-TPD and O2-TPD. XPS results showed that the increased content of Ce3+ and Mn4+ in the Fe5Mn/CeO2 catalyst promoted the formation of oxygen vacancies and unsaturated chemical bonds, providing more active sites, thus facilitating the efficient removal of NO and toluene at low temperatures. Compared with other catalysts, H2-TPR, NH3-TPD and O2-TPD indicate that Fe5Mn/CeO2 catalyst has great redox ability, stronger acidity and better oxygen migration ability. In addition, this paper explores the effects between selective catalytic reduction (NH3-SCR) and catalytic oxidation reaction of toluene over Fe5Mn/CeO2 catalyst. NH3 preferentially reacts with the active site on the catalyst to inhibit the toluene oxidation process, while NO promotes the toluene removal process. Toluene can promote the NH3-SCR process in a certain temperature range. While NO promotes the formation of NO2, NO2 effectively promotes the combination of toluene and active sites, which is conducive to the catalytic oxidation of toluene; The inhibition of toluene on the NH3-SCR process weakens with the increase of temperature. At 100 ℃, the inhibition of toluene on the NH3-SCR process disappears. When the temperature exceeds 225 ℃, toluene reacts with NO as a reducing agent and promotes the formation of NO2, thus promoting the NH3-SCR reaction.
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Key words:
- multi-pollutant control /
- NO /
- low-temperature activity /
- NH3-SCR /
- toluene /
- catalytic oxidation
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图 1 Mn/CeO2和FexMn/CeO2（x=4、5、6）催化剂同时进行NH3-SCR反应和甲苯催化氧化反应
Figure 1 Mn/CeO2 and FexMn/CeO2 (x=4, 5, 6) catalysts for simultaneous NH3-SCR reaction and toluene catalytic oxidation reaction (a): conversion of NO; (b): conversion of toluene
图 2 （a）Mn/CeO2和（b）Fe5Mn/CeO2催化剂同时脱硝与脱甲苯反应的产物分布
Figure 2 Product distribution of simultaneous de-nitrification and de-toluene reaction on (a) Mn/CeO2 and (b) Fe5Mn/CeO2 catalysts
图 3 Mn/CeO2、FexMn/CeO2（x=4、5、6）催化剂的（a）N2吸附-脱吸等温曲线和（b）孔径分布
Figure 3 Mn/CeO2 and FexMn/CeO2 (x=4, 5, 6) catalysts for (a) N2 adsorption/desorption isotherms and (b) pore size distributions
图 4 （a）Mn/CeO2和（b）Fe5Mn/CeO2催化剂的SEM照片和EDS-mapping照片
Figure 4 SEM and EDS mapping of (a) Mn/CeO2 and (b) Fe5Mn/CeO2 catalyst
图 5 Mn/CeO2和FexMn/CeO2（x=4、5、6）催化剂的XRD谱图
Figure 5 XRD patterns of Mn/CeO2 and FexMn/CeO2 (x=4, 5, 6)
图 6 Mn/CeO2、Fe5Mn/CeO2和Fe5Mn/CeO2(used)催化剂的XPS谱图
Figure 6 XPS spectra of Mn/CeO2, Fe5Mn/CeO2 and Fe5Mn/CeO2(used)(a): O 1s; (b): Ce 3d; (c): Mn 2p; (d): Fe 2p
图 7 Mn/CeO2和FexMn/CeO2（x=4、5、6）催化剂的H2-TPR谱图
Figure 7 H2-TPR patterns of Mn/CeO2 and FexMn/CeO2 (x=4, 5, 6)
图 8 Mn/CeO2和FexMn/CeO2（x=5、6）催化剂的NH3-TPD谱图
Figure 8 NH3-TPD patterns of Mn/CeO2 and FexMn/CeO2 (x=5, 6)
图 10 水蒸气对Fe5Mn/CeO2催化剂的同时脱硝与脱甲苯活性的影响
Figure 10 Effect of H2O(g) on the activity of Fe5Mn/CeO2 catalyst for simultaneous denitration and toluene removal
表 1 Mn/CeO2和FexMn/CeO2（x=4、5、6）催化剂的比表面积、孔容积和平均孔径
Table 1 Specific surface area, pore volume and average pore size of CeO2 and FexMn/CeO2 (x=4, 5, 6)
Catalyst BET surface
area A /(m2·g−1)Pore volume
v /(cm3·g−1)Pore size
d /nmMn/CeO2 23.7 0.065 7.9 Fe4Mn/CeO2 20.8 0.051 7.6 Fe5Mn/CeO2 22.1 0.052 7.2 Fe6Mn/CeO2 20.1 0.041 6.4 
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表 2 催化剂的元素组成
Table 2 Element composition of catalysts.
Catalyst Oα/Oβ Ce4 + /Ce3 + Mn4 + /（Mn3 + + Mn2 + ） Fe3 + /Fe2 + Mn/CeO2 0.84 4.26 0.419 – Fe5Mn/CeO2 1.05 4.59 0.708 2.15 Fe5Mn/CeO2(used) 0.86 6.38 0.521 1.10
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