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Mn/Fe负载活性炭低温脱硝协同脱汞实验研究

潘磊 卢平 宋涛 黄震

潘磊, 卢平, 宋涛, 黄震. Mn/Fe负载活性炭低温脱硝协同脱汞实验研究[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2022041
引用本文: 潘磊, 卢平, 宋涛, 黄震. Mn/Fe负载活性炭低温脱硝协同脱汞实验研究[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2022041
PAN Lei, LU Ping, SONG Tao, HUANG Zhen. Experimental study on low temperature NO reduction and Hg0 removal of activated carbon loaded by Mn/Fe oxides[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2022041
Citation: PAN Lei, LU Ping, SONG Tao, HUANG Zhen. Experimental study on low temperature NO reduction and Hg0 removal of activated carbon loaded by Mn/Fe oxides[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2022041

Mn/Fe负载活性炭低温脱硝协同脱汞实验研究

doi: 10.19906/j.cnki.JFCT.2022041
详细信息
    通讯作者:

    Tel: 025-85481085, Fax: 025-85481124, E-mail: luping@njnu.edu.cn

  • 中图分类号: X511

Experimental study on low temperature NO reduction and Hg0 removal of activated carbon loaded by Mn/Fe oxides

  • 摘要: 采用等体积浸渍法制备了Mn/Fe负载椰壳活性炭碳基催化剂Mn-Fe/HAC。在固定床实验台上研究了反应温度、体积空速(GHSV)和烟气组分(O2、CO、SO2和Hg0)对其脱硝脱汞性能的影响,并结合N2吸附-脱附、NH3-TPD、H2-TPR、Hg-TPD以及瞬态反应测试,分析其脱硝脱汞机理。结果表明,Mn/Fe负载可以明显促进碳基催化剂低温脱硝活性,添加Fe可提高催化剂表面的酸性位点数量和还原能力,促进催化剂活性,进一步拓宽其脱硝温度窗口;7Mn0.5Fe/HAC催化剂在160−220 ℃下的脱硝效率可达95%,且在100−220 ℃下Mn和Fe负载碳基催化剂脱汞效率基本稳定在100%。7Mn0.5Fe/HAC催化剂脱硝效率随着GHSV增加而逐渐降低,而脱汞效率则保持稳定。无O2条件下Mn/Fe催化剂脱硝较低(约为50%),而当烟气中O2含量大于6%,其脱硝效率可稳定在95%以上。Hg0浓度对Mn/Fe负载碳基催化剂脱硝性能影响不大,CO有一定抑制作用,而高浓度SO2抑制作用较为显著。Mn和Fe共负载可提高抗硫性,在含150 μL·L−1 SO2模拟烟气下,7Mn0.5Fe/HAC催化剂在180 ℃的脱硝效率仍可稳定在80%以上。烟气中NO存在能促进Hg0脱除,NH3存在则具有一定的抑制作用。Mn/Fe负载碳基催化剂脱硝遵循E-R机理,即NH3先吸附于活性位点,再与气态NO反应,最终将NO还原为N2;而脱汞遵循L-H机理,即Hg0先吸附于活性位点,形成吸附态Hg0,然后与活性氧以及吸附态NO2与SO2反应分别生成HgO、Hg(NO3)2和HgSO4
  • 图  1  催化剂制备流程图

    Figure  1  The preparation procedure of Mn/Fe modified carbon-based catalysts

    图  2  固定床烟气脱硝脱汞实验装置

    Figure  2  Experimental setup of fixed-bed reactor for NO reduction and Hg0 removal

    图  3  温度对碳基催化剂脱硝脱汞性能的影响

    Figure  3  Effects of reaction temperature on simultaneous removal of NO and Hg0 over carbon-based catalysts: (a) NO removal efficiency; (b) Hg0 removal efficiency

    图  4  GHSV对碳基催化剂脱硝脱汞性能的影响

    Figure  4  Effects of GHSV on NO and Hg0 removal over carbon-based catalysts

    图  5  O2浓度对碳基催化剂脱硝脱汞性能的影响

    Figure  5  Effects of O2 content on NO and Hg0 removal efficiency over carbon-based catalysts

    图  6  CO浓度对碳基催化剂脱硝脱汞性能的影响

    Figure  6  Effects of CO concentration on NO and Hg0 removal efficiency over carbon-based catalysts

    图  7  SO2浓度对碳基催化剂脱硝脱汞性能的影响

    Figure  7  Effects of SO2 content on NO and Hg0 removal efficiency over carbon-based catalysts

    图  8  Hg0浓度对催化剂脱硝性能影响

    Figure  8  Effects of Hg0 concentration on NO removal efficiency over carbon-based catalysts

    图  9  碳基催化剂的NH3-TPD谱图

    Figure  9  NH3-TPD profiles of carbon-based catalysts

    图  10  碳基催化剂的H2-TPR谱图

    Figure  10  H2-TPR profiles of carbon-based catalysts

    图  11  7Mn0.5Fe/HAC催化剂SCR的瞬态响应过程:(a) NH3; (b) NO

    Figure  11  Transient response during SCR process over 7Mn0.5Fe/HAC: (a) NH3; (b) NO

    图  12  7Mn0.5Fe/HAC(O)和7Mn0.5Fe/HAC(S)催化剂的Hg程序升温曲线

    Figure  12  Hg-TPD profiles of 7Mn0.5Fe/HAC(O) and 7Mn0.5Fe/HAC(S)

    表  1  椰壳活性炭的理化特性参数

    Table  1  The parameters of physiochemical property of CAC

    CarrierBET surface areaAshParticle sizeElemental analysis (wt%)
    m2·g−1wt%MeshCHONS
    CAC515.1155−871.792.0225.780.320.09
    下载: 导出CSV

    表  2  模拟烟气组分

    Table  2  Simulated flue gas composition

    O2CO2NONH3SO2COHg0N2
    % % μL·L−1 μL·L−1 μL·L−1 μL·L−1 μg·m−3 %
    6−16 12 400 400 ~150 ~8000 ~90 Balance gas
    下载: 导出CSV

    表  3  碳基催化剂的比表面积及孔结构参数

    Table  3  Specific surface area and pore structure parameters of carbon-based catalysts

    Carbon-based catalystsBET surface area
    m2·g−1
    Total pore volume
    cm3·g−1
    Average pore diameter
    nm
    HAC441.60.1861.051
    0.5Fe/HAC511.90.2370.483
    1Fe/HAC535.60.2400.503
    7Mn/HAC502.60.2331.051
    7Mn0.5Fe/HAC502.30.2151.051
    7Mn/HAC(S)437.10.1920.548
    7Mn0.5Fe/HAC(S)427.60.1930.483
    下载: 导出CSV
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  • 收稿日期:  2022-04-06
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