锑掺杂对钒钛系催化剂低温脱硝活性的影响

张铁军; 李坚; 何洪; 梁文俊; 梁全明

锑掺杂对钒钛系催化剂低温脱硝活性的影响

北京工业大学区域大气复合污染防治北京市重点实验室, 北京 100124

详细信息

通讯作者:
李坚, Tel:13801027125, E-mail:ljian@bjut.edu.cn

中图分类号: O643
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- 被引次数: 0
出版历程
- 收稿日期: 2017-02-21
- 修回日期: 2017-04-19
- 网络出版日期: 2021-01-23
- 刊出日期: 2017-06-10

Effect of antimony doped vanadium-titanium catalyst on low-temperature NH₃-SCR activity

Key Laboratory of Beijing on Regional Air Pollution Control, Beijing University of Technology, Beijing 100124, China

摘要

摘要: 用浸渍法制备Sb-V₂O₅-TiO₂催化剂，在质量分数3%V₂O₅-TiO₂催化剂基础上，研究锑的负载量、焙烧温度对催化剂活性的影响。结果表明，锑的负载量为11%（质量分数），500 ℃焙烧的催化剂具有最佳的SCR活性，在进口浓度为0.07% NO_x、O₂体积分数5%、空速27 000 h^-1的条件下，170 ℃时脱硝活性可达92%。对催化剂进行H₂-TPR表征，发现锑修饰后的催化剂氧化能力增强，使催化剂效率上升。通过XPS和NH₃-TPD表征测试，催化剂表面的锑主要以五价的形式存在且随着锑负载量的增加催化剂表面酸性增强。考察SO₂和H₂O对催化剂的影响发现，加锑催化剂具有一定的抗硫抗水性能。通过FT-IR、TG、孔隙结构测试表明，锑的加入可以有效地抑制硫酸铵盐在催化剂表面的聚集，从而延长催化剂的寿命。
- 低温 /
- SCR /
- 抗硫 /
- 硫酸铵盐
Abstract: Sb-V₂O₅-TiO₂ catalysts were prepared by wet impregnation method. The effect of antimony loadings and calcination temperatures on the activity of catalysts were investigated on the basis of 3%V₂O₅-TiO₂. The results indicate that the catalyst with 11% Sb loading, calcined at 500℃, has the best activity of SCR. The NO_x conversion could reach 92% at 170℃ with the inlet NO_x concentration of 0.07%, the O₂ volume fraction of 5%, and the space velocity of 27 000 h^-1. The H₂-TPR data reveal that the increase of activity can be attributed to the promotion of the catalyst oxidation ability by the modifying of antimony. Sb is mainly in the pentavalent antimony form on the surface of the catalyst, and the increase in surface acidity of the catalyst is identified by means of XPS and NH₃-TPD. The effects of SO₂ and H₂O on the catalyst is also studied, showing that the Sb-V₂O₅-TiO₂ has an excellent catalytic activity in the presence of H₂O and SO₂. FT-IR, TG and pore structure test results suggest that the addition of Sb can effectively inhibit the aggregation of ammonium sulfate on the catalyst surface, thereby improving the service life of the catalyst.
- low-temperature /
- SCR /
- sulfur resistance /
- ammonium sulfate

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图 1 锑的负载量对催化剂活性的影响

Figure 1 Effect of Sb loading on the activity of 3%V₂O₅-TiO₂

reaction condition: 0.07% NO_x, 0.07% NH₃, 5% O₂, N₂ balance, GHSV = 27000h^-1

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图 2 不同锑含量催化剂的H₂-TPR谱图

Figure 2 H₂-TPR profiles of Sb-V₂O₅-TiO₂ with different Sb loadings

a: 12%; b: 11%; c: 8%; d: 5%; e: 3%

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图 3 催化剂的XPS谱图

Figure 3 XPS profiles of Sb-V₂O₅-TiO₂

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图 4 催化剂的NH₃-TPD谱图

Figure 4 NH₃-TPD profiles of Sb-V₂O₅-TiO₂ and V₂O₅-TiO₂

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图 5 不同焙烧温度对催化剂活性的影响

Figure 5 Effect of calcination temperature on the activity of Sb-V₂O₅-TiO₂

reaction condition: 0.07% NO_x, 0.07% NH₃,5% O₂, N₂ balance, GHSV = 27000h^-1

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图 6 不同焙烧温度下催化剂的XRD谱图

Figure 6 XRD patterns of Sb-V₂O₅-TiO₂ with different calcination temperatures

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图 7 SO₂对V₂O₅-TiO₂和11%Sb-V₂O₅-TiO₂催化剂活性的影响

Figure 7 Effect of SO₂ on the activity of V₂O₅-TiO₂ and 11%Sb-V₂O₅-TiO₂

reaction condition: 0.07% NO_x, 0.07% NH₃, 0.03% SO₂, 5% O₂, N₂ balance, GHSV = 27000h^-1

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图 8 SO₂和H₂O对V₂O₅-TiO₂和11%Sb-V₂O₅-TiO₂催化剂脱硝活性的影响

Figure 8 Effect of SO₂ and H₂O on the activity of V₂O₅-TiO₂ and 11%Sb-V₂O₅-TiO₂

reaction condition: 0.07% NO_x, 0.07% NH₃,0.03% SO₂, 5% O₂, 10%H₂O, N₂ balance, GHSV = 27000h^-1

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图 9 催化剂抗硫抗水前后的FT-IR谱图

Figure 9 FT-IR spectra of different catalysts

a: V₂O₅-TiO₂; b: V₂O₅-TiO₂(SO₂, H₂O); c: Sb-V₂O₅-TiO₂; d: Sb-V₂O₅-TiO₂(SO₂, H₂O)

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图 10 催化剂抗硫抗水后的热重分析

Figure 10 TG analysis of different catalysts after poisoning

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表 1 催化剂的孔隙结构和H₂-TPR表征

Table 1 Pore structure parameters and H₂-TPR results

表 2 不同焙烧温度下催化剂的孔隙结构

Table 2 Catalyst pore structure parameters at different calcination temperature

表 3 中毒前后催化剂的孔隙结构

Table 3 Pore structure parameters of catalyst before and after poisoning

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