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摘要: 采用浸渍法、溶胶凝胶法和水热法制备了一系列V-Mo/TiO2催化剂，考察了制备方法对催化剂脱硝性能及抗SO2/H2O性能的研究。并运用XRD、BET、NH3-TPD、H2-TPR、XPS等方法对催化剂的理化性能进行了表征，结果表明，溶胶凝胶法制备的催化剂具有较小的晶粒粒径，较大的比表面积和孔容，较多的表面酸量，较强的氧化还原能力以及较高的V4+和表面活性氧，因此，3% V2O5-6% MoO3/TiO2（sol-gel）催化剂在80-360℃，表现出最佳的脱硝效率；引入10% H2O和0.03% SO2后，NO转化率仅下降7个百分点，表现出最佳的抗SO2/H2O性能。
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关键词:
- 催化剂 /
- V2O5-MoO3/TiO2 /
- 制备方法 /
- 脱硝效率
Abstract: A series of V-Mo/TiO2 catalysts were prepared by impregnation method, sol-gel method and hydrothermal method. The denitrification performance and anti-SO2/H2O performance of the catalysts were investigated.The physical and chemical properties of the catalyst were characterized by XRD, BET, NH3-TPD, H2-TPR and XPS.The results showed that the catalyst prepared by sol-gel method had smaller grain size, larger specific area and pore volume, more surface acidity, stronger redox ability and higher V4+ and surface active oxygen.Therefore, the 3% V2O5-6% MoO3/TiO2 (sol-gel) catalyst exhibited the best denitration efficiency in the temperature range of 80-360℃. After introducing 10% H2O and 0.03% SO2, the NO conversion of 3% V2O5-6% MoO3/TiO2 (sol-gel) catalyst decreased by only 7 percentage points, showing the best resistance to SO2/H2O.-
Key words:
- catalyst /
- V2O5-MoO3/TiO2 /
- preparation method /
- denitration efficiency
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图 3 SO2对催化剂脱硝活性的影响
Figure 3 Effect of SO2 on the denitrification activity of the catalyst
图 4 SO2和H2O对催化剂脱硝活性的影响
Figure 4 Effect of SO2 and H2O on the denitrification activity of the catalyst
图 8 催化剂的XPS谱图
Figure 8 XPS spectra of the catalyst
(a): V 2p; (b): Mo 3d; (c): O 1s; (d): correlation between Oα/(Oα+Oβ) and catalyst reaction rate constant (k) at 140℃
表 1 催化剂的结构和晶胞参数
Table 1 Structure and unit cell parameters of the catalyst
Sample Crystal parameters /nm D/nm v/nm3 a b c IM 0.378116 0.378116 0.949616 29.53 0.13577 Sol-gel 0.377498 0.377498 0.950567 13.07 0.13546 HTM 0.376812 0.376812 0.946093 30.29 0.13433 
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表 2 催化剂的物理化学性质
Table 2 Physicochemical properties of the catalyst
Sample Specific surface area
A/(m2·g-1)Average pore volume
v/(cm3·g-1)Average aperture
d/nmH2 consumption
/(μmol·g-1)IM 61.7 0.124 7.27 224 Sol-gel 65.4 0.172 7.13 599 HTM 63.7 0.158 7.02 315
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表 3 催化剂的酸量分布
Table 3 Acid distribution of catalyst
Sample Weak acid /
total acid(%)Total acid
(normalized calculation)IM 0.48 1 Sol-gel 0.68 10.94 HTM 0.60 1.46
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表 4 催化剂的表面原子浓度
Table 4 Surface atomic concentration of the catalyst
Sample O 1s E/eV V 2p E/eV Mo 3d E/eV Oα/
(Oα+Oβ)V4+/
(V4++V5+)Mo4+/
(Mo4++Mo6+)Oα Oβ V4+ V5+ 3d5/2 3d3/2 Mo4+ Mo6+ Mo4+ Mo6+ IM 530.4 531.8 516.8 517.5 232.6 233.1 235.9 236.3 0.32 0.36 0.21 Sol-gel 530.4 531.8 516.7 517.5 232.7 233.2 235.9 236.3 0.36 0.39 0.17 HTM 530.3 531.3 516.9 517.5 232.6 233.0 235.7 236.2 0.34 0.31 0.20
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