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平板式V2O5-MoO3/TiO2型SCR催化剂的中低温脱硝和抗中毒性能研究

蔺卓玮 陆强 唐昊 李慧 董长青 杨勇平

蔺卓玮, 陆强, 唐昊, 李慧, 董长青, 杨勇平. 平板式V2O5-MoO3/TiO2型SCR催化剂的中低温脱硝和抗中毒性能研究[J]. 燃料化学学报(中英文), 2017, 45(1): 113-122.
引用本文: 蔺卓玮, 陆强, 唐昊, 李慧, 董长青, 杨勇平. 平板式V2O5-MoO3/TiO2型SCR催化剂的中低温脱硝和抗中毒性能研究[J]. 燃料化学学报(中英文), 2017, 45(1): 113-122.
LIN Zhuo-wei, LU Qiang, TANG Hao, LI Hui, DONG Chang-qing, YANG Yong-ping. Research on the middle-low temperature denitration and anti-poisoning properties of plate V2O5-MoO3/TiO2 SCR catalysts[J]. Journal of Fuel Chemistry and Technology, 2017, 45(1): 113-122.
Citation: LIN Zhuo-wei, LU Qiang, TANG Hao, LI Hui, DONG Chang-qing, YANG Yong-ping. Research on the middle-low temperature denitration and anti-poisoning properties of plate V2O5-MoO3/TiO2 SCR catalysts[J]. Journal of Fuel Chemistry and Technology, 2017, 45(1): 113-122.

平板式V2O5-MoO3/TiO2型SCR催化剂的中低温脱硝和抗中毒性能研究

基金项目: 

国家重点基础研究发展规划 973 project

国家重点基础研究发展规划 2015CB251501

中央高校基本科研业务费 2016YQ05

中央高校基本科研业务费 2015ZZD02

详细信息
    通讯作者:

    陆强, Tel:010-61772030, E-mail:qianglu@mail.ustc.edu.cn

  • 中图分类号: X51

Research on the middle-low temperature denitration and anti-poisoning properties of plate V2O5-MoO3/TiO2 SCR catalysts

Funds: 

Major State Basic Research Development Program of China 973 project

Major State Basic Research Development Program of China 2015CB251501

Fundamental Research Funds for the Central Universities 2016YQ05

Fundamental Research Funds for the Central Universities 2015ZZD02

  • 摘要: 针对中低温锅炉烟气脱硝技术需求的特点,采用等体积浸渍法,以V2O5为活性组分、MoO3为助剂,制备了高钒高钼含量的V2O5-MoO3/TiO2型粉末和平板式SCR脱硝催化剂,考察了活性组分和助剂含量对催化剂活性以及抗SO2和H2O中毒性能的影响,对反应前后的催化剂进行了微观表征,并针对最优催化剂研究了其在不同烟气工况下催化剂的脱硝性能。结果表明,提升V2O5负载量可以有效提高催化剂的脱硝活性;MoO3助剂的添加也可以提高催化剂的脱硝活性。XPS、XRF、FT-IR等表征结果表明,MoO3的含量会影响催化剂中V4+/V5+的比值,其相对含量的增加有利于催化剂中非化学计量钒物种的形成以及化学吸附氧比例的增加,钼与钒物种间的交互作用是抑制SO2和H2O对催化剂的毒化作用的关键。3V2O5-10MoO3/TiO2平板式催化剂在温度为200℃、空速为3 500 h-1含SO2和H2O烟气条件下,经30 d连续反应,脱硝效率稳定维持在82%左右,该催化剂在中低温下具有优异的抗SO2和H2O中毒性能以及稳定性。
  • 图  1  SCR脱硝实验装置示意图

    Figure  1  Schematic diagram of the SCR experimental setup

    图  2  V2O5和MoO3负载量对催化剂脱硝效率的影响

    Figure  2  Effects of V2O5(a) and MoO3(b) loadings on denitrification efficiency of the catalysts

    图  3  SO2和H2O对F-3V2O5-10MoO3/ TiO2、F-5V2O5-10MoO3/TiO2、F-5V2O5-10WO3/TiO2催化剂的影响

    Figure  3  NOx conversions over F-3V2O5-10MoO3/ TiO2, F-5V2O5-10MoO3/TiO2 and F-5V2O5-10WO3/TiO2 catalysts in the presence of SO2 and H2O (temperature 200 ℃, space velocity 24 000 h-1, NH3/NO (volume ratio)=1.0)

    图  4  SO2和H2O对B-3V2O5-10MoO3/TiO2与B-5V2O5-10MoO3/ TiO2催化剂的影响

    Figure  4  NOx conversions over B-3V2O5-10MoO3/ TiO2 and B-5V2O5-10MoO3/TiO2 catalysts in the presence of SO2 and H2O (temperature 200 ℃, space velocity 3 500 h-1, NH3/NO (volume ratio)=1.0)

    图  5  新鲜催化剂和反应后催化剂的V 2p3/2 XPS谱图

    Figure  5  V 2p3/2 XPS spectra of the fresh catalysts (a) and used catalysts (b)

    图  6  新鲜催化剂和反应后催化剂的Mo 3d XPS谱图

    Figure  6  Mo 3d XPS spectra of the fresh catalysts (a) and used catalysts (b)

    图  7  新鲜催化剂和反应后催化剂的O 1s XPS谱图

    Figure  7  O 1s XPS spectra of the fresh catalysts (a) and used catalysts (b)

    图  8  反应后催化剂的S 2p3/2 XPS谱图

    Figure  8  S 2p 3/2 XPS spectra of the used catalysts

    图  9  新鲜催化剂和反应后催化剂的FT-IR谱图

    Figure  9  FT-IR spectra of the fresh and used catalysts

    图  10  温度、NOx浓度、SO2浓度、空速对B-3V2O5-10MoO3/TiO2催化剂脱硝效率的影响

    Figure  10  Effects of temperature (a), NOx concentration (b), SO2 concentration (c), space velocity (d) on denitrification efficiency over B-3V2O5-10MoO3/TiO2 catalyst

    表  1  催化剂的比表面积和孔结构

    Table  1  Specific surface area and pore structure of the catalysts

    SampleCatalystSpecific surface area
    A/(m2·g-1)
    Pore volume
    v/(cm3·g-1)
    Average pore diameter
    d/nm
    1F-3V2O5-10MoO3/TiO2(fresh)71.430.3217.8
    2F-5V2O5-10MoO3/TiO2(fresh)50.640.2519.6
    3B-3V2O5-10MoO3/TiO2(fresh)54.320.2316.7
    4B-5V2O5-10MoO3/TiO2(fresh)49.040.2218.0
    5F-3V2O5-10MoO3/TiO2(after SCR)62.090.2818.0
    6F-5V2O5-10MoO3/TiO2(after SCR)35.780.1719.9
    7B-3V2O5-10MoO3/TiO2(after SCR)*26.640.1624.4
    8B-5V2O5-10MoO3/TiO2(after SCR)38.140.1819.3
    *duration time of the SO2 and H2O deactivation experiment: NO.5 and NO.6 catalysts were 167 h, NO.7 catalyst was 120 d and NO.8 catalyst was 17 d
    下载: 导出CSV

    表  2  催化剂中各组分含量

    Table  2  Each component content of the catalysts

    SampleContent w/%
    V2O5MoO3SiO2Al2O3SO3TiO2
    12.868.66---88.27
    24.988.62---86.22
    32.708.046.595.37-75.82
    44.807.966.385.18-74.39
    52.808.46--1.6486.19
    64.748.25--5.4380.70
    72.517.336.214.498.4769.06
    84.347.546.254.934.5271.45
    *: annotation: duration time of the SO2 and H2O deactivation experiment: NO.5 and NO.6 catalysts were 167 h, NO.7 catalyst was 120 d and NO.8 catalyst was 17 d
    下载: 导出CSV
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  • 收稿日期:  2016-08-29
  • 修回日期:  2016-11-16
  • 网络出版日期:  2021-01-23
  • 刊出日期:  2017-01-10

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