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Effect of Fe2O3 on ZrTiO4 support for NH3-SCR catalytic performance

YUAN Long-teng HU Ping HU Bo-liang HAN Jia-yu MA Sheng-jie YANG Fan

袁龙腾, 胡平, 胡卜亮, 韩嘉彧, 马升捷, 杨帆, Alex A. Volinsky. Fe2O3对ZrTiO4载体NH3-SCR催化性能的影响[J]. 燃料化学学报(中英文), 2023, 51(12): 1843-1855. doi: 10.1016/S1872-5813(23)60377-9
引用本文: 袁龙腾, 胡平, 胡卜亮, 韩嘉彧, 马升捷, 杨帆, Alex A. Volinsky. Fe2O3对ZrTiO4载体NH3-SCR催化性能的影响[J]. 燃料化学学报(中英文), 2023, 51(12): 1843-1855. doi: 10.1016/S1872-5813(23)60377-9
YUAN Long-teng, HU Ping, HU Bo-liang, HAN Jia-yu, MA Sheng-jie, YANG Fan, . Effect of Fe2O3 on ZrTiO4 support for NH3-SCR catalytic performance[J]. Journal of Fuel Chemistry and Technology, 2023, 51(12): 1843-1855. doi: 10.1016/S1872-5813(23)60377-9
Citation: YUAN Long-teng, HU Ping, HU Bo-liang, HAN Jia-yu, MA Sheng-jie, YANG Fan, . Effect of Fe2O3 on ZrTiO4 support for NH3-SCR catalytic performance[J]. Journal of Fuel Chemistry and Technology, 2023, 51(12): 1843-1855. doi: 10.1016/S1872-5813(23)60377-9

Fe2O3对ZrTiO4载体NH3-SCR催化性能的影响

doi: 10.1016/S1872-5813(23)60377-9
详细信息
  • 中图分类号: O643.36

Effect of Fe2O3 on ZrTiO4 support for NH3-SCR catalytic performance

Funds: The project was supported by the Scientific and Technological Innovation Team Project of the Shaanxi Innovation Capability Support Plan, China (2022TD-30), the Youth Innovation Team of Shaanxi Universities (2019-2022), the Top Young Talents Project of “Special support program for high-level talents” in the Shaanxi Province (2018-2023), and the International Science and Technology Cooperation Program of the Shaanxi Province (2022KW-39), Xi’an Science and Technology Planning Project (2022JH-RYFW-0196)
More Information
  • 摘要: NH3-SCR催化剂主要用于工业生产和汽车尾气清洁,本研究采用“共沉淀-浸渍法”制备了新型α%Fe2O3/ZrTiO4(α=0、8、12、15)催化剂。结果表明,α%Fe2O3/ZrTiO4催化剂的最佳成分配比的12%Fe2O3/ZrTiO4催化剂在250−400 ℃条件下NOx转化率大于80%,在300 ℃时NOx转化率接近100%,并且N2选择性在200−450 ℃大于90%。在ZrTiO4表面负载Fe2O3后,催化剂的氧化还原性能、表面酸度和Oβ/(Oα + Oβ)比例都有所提高,这不仅归因于α%Fe2O3/ZrTiO4催化剂具有多孔结构,还归因于活性组分Fe2O3和载体ZrTiO4之间的电子相互作用。此外,原位DRIFTs反应表明,12%Fe2O3/ZrTiO4催化剂的NH3-SCR反应遵循Eley-Rideal机制。明确的反应机制有利于更深入了解SCR过程中NOx转化的反应过程。这项工作为未来Fe基SCR催化剂在中温范围内替代V基催化剂提供了可行的策略。
  • FIG. 2811.  FIG. 2811.

    FIG. 2811.  FIG. 2811.

    Figure  1  SEM images of ZrTiO4 and α%Fe2O3/ZrTiO4 samples (a): ZrTiO4; (b): 8%Fe2O3/ZrTiO4; (c): 12%Fe2O3/ZrTiO4; (d): 15%Fe2O3/ZrTiO4

    Figure  2  Adsorption isotherms of ZrTiO4 and α%Fe2O3/ZrTiO4 samples (The curves are offset for clarity and are plotted with the same y scale)

    Figure  3  XRD patterns of ZrTiO4 and α%Fe2O3/ZrTiO4 samples

    Figure  4  (a) SEM image and EDX elemental maps of the 12%Fe2O3/ZrTiO4 catalyst: (b) Zr, (c) Fe and (d) Ti

    Figure  5  NH3-TPD profiles of ZrTiO4 and α% Fe2O3/ZrTiO4 samples

    Figure  6  H2-TPR profiles of ZrTiO4 and α% Fe2O3/ZrTiO4 samples

    Figure  7  (a) NOx conversion of ZrTiO4 and α%Fe2O3/ZrTiO4 samples; (b) N2 selectivity; (c) NH3 conversion; (d) N2O emissions (Reactant feed contains 5.0×10−4 of NO, 6.0×10−4 of NH3, 3%O2 balanced with N2)

    Figure  8  XPS profiles of ZrTiO4 and α%Fe2O3/ZrTiO4 samples: (a) Ti 2p; (b) Zr 3d; (c) Fe 2p; (d) O 1s

    Figure  9  DRIFT spectra of (a) NH3 adsorption and (b) NO + O2 adsorption on 12%Fe2O3/ZrTiO4 catalyst at different temperatures

    Figure  10  DRIFT spectra of reaction between (a) pre-adsorption of NH3 and NO + O2 (b) pre-adsorption of NO + O2 and NH3 on 12%Fe2O3/ZrTiO4 catalyst

    Figure  11  Reaction mechanism of 12%Fe2O3/ZrTiO4 catalyst

    Table  1  SBET surface area, pore volume and pore size of ZrTiO4 and α%Fe2O3/ZrTiO4 samples

    SampleSurface area
    / (m2·g−1)
    Pore volume
    /(cm3·g−1)
    Pore size
    /nm
    ZrTiO4161.30.8521.19
    8%Fe2O3/ZrTiO4134.30.5014.87
    12%Fe2O3/ZrTiO4139.60.7722.02
    15%Fe2O3/ZrTiO4129.10.5817.92
    下载: 导出CSV

    Table  2  XPS concentration of ZrTiO4 and α%Fe2O3/ZrTiO4

    SampleAtomic concentrationRelative concentration /%
    FeZrTiOOβ/(Oα + Oβ)Fe3+ /(Fe3+ + Fe2+ )
    ZrTiO414.415.370.323.1
    8%Fe2O3/ZrTiO41.8513.313.271.634.043
    12%Fe2O3/ZrTiO42.2113.312.871.631.773.4
    15%Fe2O3/ZrTiO42.6813.213.171.028.791.7
    下载: 导出CSV
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  • 收稿日期:  2023-03-15
  • 修回日期:  2023-04-08
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  • 网络出版日期:  2023-06-27
  • 刊出日期:  2023-12-05

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