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不同分子筛负载锰铈催化剂的低温NH3-SCR脱硝性能

黄增斌 李翠清 王振 徐胜美 冯凌波 王虹 宋永吉 张伟

黄增斌, 李翠清, 王振, 徐胜美, 冯凌波, 王虹, 宋永吉, 张伟. 不同分子筛负载锰铈催化剂的低温NH3-SCR脱硝性能[J]. 燃料化学学报(中英文), 2016, 44(11): 1388-1393.
引用本文: 黄增斌, 李翠清, 王振, 徐胜美, 冯凌波, 王虹, 宋永吉, 张伟. 不同分子筛负载锰铈催化剂的低温NH3-SCR脱硝性能[J]. 燃料化学学报(中英文), 2016, 44(11): 1388-1393.
HUANG Zeng-bin, LI Cui-qing, WANG Zhen, XU Sheng-mei, FENG Ling-bo, WANG Hong, SONG Yong-ji, ZHANG Wei. Performance of Mn-Ce catalysts supported on different zeolites in the NH3-SCR of NOx[J]. Journal of Fuel Chemistry and Technology, 2016, 44(11): 1388-1393.
Citation: HUANG Zeng-bin, LI Cui-qing, WANG Zhen, XU Sheng-mei, FENG Ling-bo, WANG Hong, SONG Yong-ji, ZHANG Wei. Performance of Mn-Ce catalysts supported on different zeolites in the NH3-SCR of NOx[J]. Journal of Fuel Chemistry and Technology, 2016, 44(11): 1388-1393.

不同分子筛负载锰铈催化剂的低温NH3-SCR脱硝性能

基金项目: 

国家自然科学基金 21343009

详细信息
    通讯作者:

    李翠清, Tel:010-81292124, E-mail:licuiqing@bipt.edu.cn

  • 中图分类号: O643

Performance of Mn-Ce catalysts supported on different zeolites in the NH3-SCR of NOx

Funds: 

the National Natural Science Foundation of China 21343009

  • 摘要: 分别以β、ZSM-5和USY分子筛为载体,采用浸渍法制备了锰铈催化剂,对其低温NH3-SCR反应性能进行了评价,并采用XRD、BET、NH3-TPD、H2-TPR以及XPS对催化剂进行了表征。结果表明,三种分子筛负载的锰铈催化剂均具有较好的低温NH3-SCR反应活性,其中,Mn-Ce/USY的催化性能最好,在107℃时NOx转化率可达到90%。负载锰铈后催化剂的比表面积和孔体积均有所下降;活性组分MnOx主要以无定型态分布于催化剂表面,且在ZSM-5上检测到聚集的CeO2。催化剂表面弱酸对低温NH3-SCR反应起主要作用,催化剂表面上活性组分的表面浓度和氧化态明显不同,较高的Mn4+/Mn3+原子比和吸附氧表面浓度对提高催化剂的低温NH3-SCR反应活性有利。
  • 图  1  不同载体负载的Mn-Ce催化剂的XRD谱图

    Figure  1  XRD patterns of the Mn-Ce catalysts supported on different zeolites

    图  2  不同载体负载的Mn-Ce催化剂的H2-TPR谱图

    Figure  2  H2-TPR profiles of Mn-Ce catalysts supported on different zeolites

    图  3  不同载体负载的Mn-Ce催化剂的NH3-TPD谱图

    Figure  3  NH3-TPD profiles of the Mn-Ce catalysts supported on different zeolites

    图  4  不同载体负载的Mn-Ce催化剂的XPS谱图

    Figure  4  XPS spectra of the Mn-Ce catalysts supported on different zeolites

    图  5  不同载体负载的Mn-Ce催化剂的NOx转化率

    Figure  5  NOx conversion for NH3-SCR over the Mn-Ce catalysts supported on different zeolites

    表  1  不同载体负载的Mn-Ce催化剂的BET及孔径

    Table  1  BET surface area and pore size distribution of the Mn-Ce catalysts supported on different zeolites

    Catalyst Pore size d/nm Pore volume v/(cm3·g-1) ABET/(m2·g-1)
    β 45.51 0.95 492.08
    Mn-Ce/β 45.76 0.87 306.74
    USY 43.22 0.86 520.35
    Mn-Ce/USY 44.06 0.79 362.27
    ZSM-5 41.44 0.73 302.25
    Mn-Ce/ZSM-5 42.99 0.69 199.38
    下载: 导出CSV

    表  2  不同载体负载的Mn-Ce催化剂的H2-TPR表征

    Table  2  H2-TPR results of the Mn-Ce catalysts supported on different zeolites

    Catalyst Temperature for the low temperature reduction peak t/℃ Area for the low temperature reduction peak
    Mn-Ce/ZSM-5 345 24.6
    Mn-Ce/USY 350 29.7
    Mn-Ce/β 340 22.9
    下载: 导出CSV

    表  3  不同载体负载的Mn-Ce催化剂的NH3-TPD表征

    Table  3  NH3-TPD results of the Mn-Ce catalysts supported on different zeolites

    Catalyst Low temperature of desorption peaks t/℃ Peak area of low temperature desorption peak
    Mn-Ce/ZSM-5 160 30.3
    Mn-Ce/USY 155 31.1
    Mn-Ce/β 157 30.6
    下载: 导出CSV

    表  4  催化剂Mn 2p3/2 XPS表征

    Table  4  Results of curve-fittings on the Mn 2p3/2 peak in XPS patterns of the Mn-Ce catalysts

    Catalyst Mn4+watom/% Mn4+EB/eV Mn3+watom/% Mn3+EB/eV Mn4+/Mn3+(atomic ratio)
    Mn-Ce/ZSM-5 59.6 642.7 40.4 641.2 1.48
    Mn-Ce/USY 92.7 642.7 7.3 641.2 12.70
    Mn-Ce/β 62.1 642.7 37.9 641.2 1.64
    下载: 导出CSV

    表  5  催化剂O 1s XPS表征

    Table  5  Results of curve-fittings on the O 1s speak in XPS patterns of the Mn-Ce catalysts

    Catalyst Chemisorbed oxygen watom/% Chemisorbed oxygen EB/eV Lattice oxygen watom/% Lattice oxygen EB/eV
    Mn-Ce/ZSM-5 73.9 532.2 26.1 529.5
    Mn-Ce/USY 95.5 532.2 4.5 529.5
    Mn-Ce/β 91.7 532.2 8.3 529.5
    下载: 导出CSV
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出版历程
  • 收稿日期:  2016-04-15
  • 修回日期:  2016-07-19
  • 网络出版日期:  2021-01-23
  • 刊出日期:  2016-11-10

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