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不同孔结构CeTiOx催化剂的制备及其NH3-SCR脱硝性能研究

谭晨晨 韩宇轩 胡亚琴 沈凯 丁世鹏 张亚平

谭晨晨, 韩宇轩, 胡亚琴, 沈凯, 丁世鹏, 张亚平. 不同孔结构CeTiOx催化剂的制备及其NH3-SCR脱硝性能研究[J]. 燃料化学学报(中英文), 2024, 52(1): 65-75. doi: 10.1016/S1872-5813(23)60369-X
引用本文: 谭晨晨, 韩宇轩, 胡亚琴, 沈凯, 丁世鹏, 张亚平. 不同孔结构CeTiOx催化剂的制备及其NH3-SCR脱硝性能研究[J]. 燃料化学学报(中英文), 2024, 52(1): 65-75. doi: 10.1016/S1872-5813(23)60369-X
TAN Chenchen, HAN Yuxuan, HU Yaqin, SHEN Kai, DING Shipeng, ZHANG Yaping. Preparation and NH3-SCR catalytic performance of CeTiOx catalysts with different pore structures[J]. Journal of Fuel Chemistry and Technology, 2024, 52(1): 65-75. doi: 10.1016/S1872-5813(23)60369-X
Citation: TAN Chenchen, HAN Yuxuan, HU Yaqin, SHEN Kai, DING Shipeng, ZHANG Yaping. Preparation and NH3-SCR catalytic performance of CeTiOx catalysts with different pore structures[J]. Journal of Fuel Chemistry and Technology, 2024, 52(1): 65-75. doi: 10.1016/S1872-5813(23)60369-X

不同孔结构CeTiOx催化剂的制备及其NH3-SCR脱硝性能研究

doi: 10.1016/S1872-5813(23)60369-X
基金项目: 国家重点研发计划(2021YFB3500604)项目资助
详细信息
    通讯作者:

    Tel: 18936874668, E-mail: amflora@seu.edu.cn

  • 中图分类号: O643.36

Preparation and NH3-SCR catalytic performance of CeTiOx catalysts with different pore structures

Funds: The project was supported by National Key Research and Development Program of China (2021YFB3500604)
  • 摘要: 为探究催化剂的孔结构对催化剂脱硝活性的影响,采用溶胶凝胶法分别制备了三维有序大孔-介孔(3DOM-m) CeTiOx、三维有序大孔(3DOM) CeTiOx、三维有序介孔(3DOm) CeTiOx及无序孔(DM) CeTiOx等四种不同孔结构的催化剂。NH3-SCR测试结果表明,催化剂活性依次为3DOM-m CeTiOx>3DOm CeTiOx>3DOM CeTiOx>DM CeTiOx,3DOM-m CeTiOx表现出更优异的催化活性,NO转化率在60000 h−1、250–400 ℃时超过90%。通过XRD、SEM、BET、NH3-TPD、in-situ DRIFTS等技术对催化剂进行表征分析。结果表明,催化剂的比表面积并不是决定CeTiOx脱硝活性的主导因素。3DOM-m CeTiOx具有高度有序的大孔-介孔结构、丰富的Brønsted酸酸性位点,进而提高了催化剂的脱硝活性。3DOM-m CeTiOx催化剂在NH3-SCR反应过程中同时遵循E-R机理和L-H机理。
  • FIG. 2881.  FIG. 2881.

    FIG. 2881.  FIG. 2881.

    图  1  不同孔结构的CeTiOx催化剂NO转化率

    Figure  1  NO conversions over CeTiOx catalysts with different pore structures

    图  2  不同孔结构CeTiOx催化剂的XRD谱图(a)及小角XRD谱图(b)

    Figure  2  XRD patterns (a) and small angle XRD patterns (b) of CeTiOx catalysts with different pore structures

    图  3  PMMA模板及CeTiOx催化剂的SEM照片

    Figure  3  SEM images of PMMA microspheres and CeTiOx catalysts

    (a): PMMA microspheres; (b), (c): 3DOM-m CeTiOx; (d): 3DOM CeTiOx; (e): 3DOm CeTiOx; (f): DM CeTiOx.

    图  4  不同孔结构 CeTiOx催化剂的氮气吸附-脱附等温线(a)及介孔分布(b)

    Figure  4  N2 adsorption-desorption isotherm (a) and mesoporous distribution (b) of CeTiOx catalysts with different pore structures

    图  5  不同孔结构CeTiOx催化剂的NH3-TPD谱图

    Figure  5  NH3-TPD profiles of CeTiOx catalysts with different pore structures

    图  6  CeTiOx催化剂表面 NH3吸附in-situ DRIFTS 谱图

    Figure  6  In situ DRIFTS of NH3 with CeTiOx catalysts at different temperatures

    (a): 3DOM-m CeTiOx; (b): 3DOM CeTiOx; (c): 3DOm CeTiOx; (d): DM CeTiOx.

    图  7  不同孔结构CeTiOx催化剂B酸、L酸量计算结果(50 ℃)

    Figure  7  Acid content (a) and amount (b) of CeTiOx catalysts with different pore structures at 50 ℃

    图  8  CeTiOx催化剂表面 NO+O2吸附 in-situ DRIFTS 谱图

    Figure  8  In situ DRIFTS of NO+O2 on CeTiOx catalysts at different temperatures

    (a): 3DOM-m CeTiOx; (b): 3DOM CeTiOx; (c): 3DOm CeTiOx; (d): DM CeTiOx.

    图  9  3DOM-m CeTiOx催化剂表面NH3吸附饱和后通NO+O2 (a), NO+O2吸附饱和后通NH3 (b) in-situ DRIFTS谱图(200 ℃)

    Figure  9  In-situ DRIFTS of NO+O2 reacting with pre-adsorbed NH3 (a), NH3 reacting with pre-adsorbed NO+O2 (b) over the 3DOM-m CeTiOx catalyst at 200 ℃

    表  1  不同孔结构CeTiOx催化剂的结构

    Table  1  Textural properties of CeTiOx catalysts with different pore structures

    CatalystSurface area
    A/(m2·g−1)
    Pore volume v/(cm3·g−1)Average pore size d/nm
    3DOM-m CeTiOx107.30.2178.1
    3DOM CeTiOx60.90.1197.4
    3DOm CeTiOx257.60.3485.4
    DM CeTiOx49.30.0977.5
    下载: 导出CSV

    表  2  不同孔结构CeTiOx催化剂的NH3-TPD计算

    Table  2  The results of NH3-TPD

    CatalystWeak acid amount/(μmol∙g−1)Medium strong acid amount/(μmol∙g−1)Total acid amount/(μmol∙g−1)
    3DOM-m CeTiOx10135136
    3DOM CeTiOx601272
    3DOm CeTiOx712697
    DM CeTiOx56863
    下载: 导出CSV
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  • 收稿日期:  2023-04-16
  • 修回日期:  2023-04-28
  • 录用日期:  2023-05-05
  • 网络出版日期:  2023-05-17
  • 刊出日期:  2024-01-09

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