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WO3-TiO2/SBA-15的制备及其光催化氧化脱硫性能

张璐璐 詹金友 孙尧 沈健

张璐璐, 詹金友, 孙尧, 沈健. WO3-TiO2/SBA-15的制备及其光催化氧化脱硫性能[J]. 燃料化学学报(中英文), 2016, 44(6): 754-762.
引用本文: 张璐璐, 詹金友, 孙尧, 沈健. WO3-TiO2/SBA-15的制备及其光催化氧化脱硫性能[J]. 燃料化学学报(中英文), 2016, 44(6): 754-762.
ZHANG Lu-lu, ZHAN Jin-you, SUN Yao, SHEN Jian. Preparation of WO3-TiO2/SBA-15 catalyst and its photocatalytic performance in oxidative desulfurization[J]. Journal of Fuel Chemistry and Technology, 2016, 44(6): 754-762.
Citation: ZHANG Lu-lu, ZHAN Jin-you, SUN Yao, SHEN Jian. Preparation of WO3-TiO2/SBA-15 catalyst and its photocatalytic performance in oxidative desulfurization[J]. Journal of Fuel Chemistry and Technology, 2016, 44(6): 754-762.

WO3-TiO2/SBA-15的制备及其光催化氧化脱硫性能

详细信息
  • 中图分类号: TQ426

Preparation of WO3-TiO2/SBA-15 catalyst and its photocatalytic performance in oxidative desulfurization

More Information
  • 摘要: 采用孔道内水解法制备了WO3-TiO2/SBA-15催化剂用于光催化氧化柴油脱硫, 利用XRD、SEM、EDS、N2吸附-脱附、FT-IR、TG-DTA和UV-vis等技术对该催化剂进行了表征, 考察了WO3和TiO2负载量、焙烧温度和焙烧时间对其光催化氧化脱硫性能的影响。结果表明, WO3和TiO2负载量分别为1.6%和15%, 焙烧温度500℃, 焙烧时间为3 h条件所制备的催化剂性能最佳; 在该条件下制备的WO3-TiO2/SBA-15催化剂仍保持SBA-15的六方介孔结构, 模拟柴油的脱硫率高达87.9%, 且具有良好的回收再生性能。
  • 图  1  WO3-TiO2/SBA-15的光催化机理示意图

    Figure  1  Proposed mechanism of photocatalytic oxidative desulfurization over the WO3-TiO2/SBA-15 catalyst

    图  2  SBA-15和1.6WO3-yTiO2/SBA-15催化剂的小角XRD谱图

    Figure  2  Small angle XRD patterns of SBA-15 and 1.6WO3-yTiO2/SBA-15 catalysts

    a: SBA-15; b: 1.6WO3/SBA-15; c: 1.6WO3-10TiO2/SBA-15; d: 1.6WO3-15TiO2/SBA-15; e: 1.6WO3-20TiO2/SBA-15

    图  3  焙烧温度为500℃时TiO2和1.6WO3-15TiO2/SBA-15催化剂的大角XRD谱图

    Figure  3  Wide angle XRD patterns of TiO2 and 1.6WO3-15TiO2/SBA-15 calcined at 500℃

    图  4  1.6WO3-15TiO2/SBA-15催化剂的SEM照片

    Figure  4  SEM photos of the 1.6WO3-15TiO2/SBA-15 catalyst

    图  5  1.6WO3-15TiO2/SBA-15催化剂的EDS照片

    Figure  5  EDS images of the 1.6WO3-15TiO2/SBA-15 catalyst

    图  6  SBA-15和1.6WO3-yTiO2/SBA-15催化剂的N2吸附-脱附谱图

    Figure  6  N2 adsorption-desorption isotherms of SBA-15 and 1.6WO3-yTiO2/SBA-15 catalysts

    a: SBA-15; b: 1.6WO3/SBA-15; c: 1.6WO3-10TiO2/SBA-15; d: 1.6WO3-15TiO2/SBA-15; e: 1.6WO3-20TiO2/SBA-15

    图  7  SBA-15和1.6WO3-15TiO2/SBA-15催化剂的孔径分布

    Figure  7  Pore size distribution of SBA-15 (a) and 1.6WO3-15TiO2/SBA-15 catalyst (b)

    图  8  SBA-15和1.6WO3-15TiO2/SBA-15催化剂的FT-IR谱图

    Figure  8  FT-IR spectra of SBA-15 (a) and 1.6WO3-15TiO2/SBA-15 (b)

    图  9  1.6WO3-15TiO2/SBA-15催化剂的TG-DTA曲线

    Figure  9  TG-DTA curves of 1.6WO3-15TiO2/SBA-15 catalyst

    图  10  15TiO2/SBA-15和1.6WO3-15TiO2/SBA-15催化剂的紫外-可见吸收光谱谱图

    Figure  10  UV-vis spectra of 15TiO2/SBA-15 (a) and 1.6WO3-15TiO2/SBA-15 (b)

    图  11  不同条件下脱硫效果的比较

    Figure  11  Desulfurization rates under different conditions

    a: UV light+H2O2; b: UV light+H2O2+WO3/TiO2; c: UV light+H2O2+SBA-15; d: UV light+H2O2+1.6WO3/SBA-15; e: UV light+H2O2+15TiO2/SBA-15+H2O2; f: H2O2+1.6WO3-15TiO2/SBA-15; g: UV light+H2O2+1.6WO3-15TiO2/SBA-15

    图  12  WO3-TiO2/SBA-15催化剂中WO3-TiO2负载量对脱硫率的影响

    Figure  12  Effect of loading amount of WO3-TiO2 in WO3-TiO2/SBA-15 sample on desulfurization rate

    图  13  焙烧温度对制备的1.6WO3-15TiO2/SBA-15催化剂脱硫率的影响

    Figure  13  Effect of calcination temperature on the desulfurization rate over the 1.6WO3-15TiO2/SBA-15 catalyst calcined for 3 h

    图  14  焙烧时间对制备的1.6WO3-15TiO2/SBA-15催化剂脱硫率的影响

    Figure  14  Effect of calcination time on the desulfurization rate over the 1.6WO3-15TiO2/SBA-15 catalyst calcined at 500℃

    图  15  催化剂重复使用次数对脱硫率的影响

    Figure  15  Desulfurization rates over the 1.6WO3-15TiO2/SBA-15 catalyst reused for different cycles

    表  1  SBA-15和1.6WO3-yTiO2/SBA-15样品的结构参数

    Table  1  Textural parameters of SBA-15 and 1.6WO3-yTiO2/SBA-15 catalysts

    SampleSurface
    area
    A/(m2·g-1)
    Pore
    volume v/
    (cm3·g-1)
    Pore
    size
    d /nm
    SBA-15876.351.096.35
    1.6WO3/SBA-15849.420.996.32
    1.6WO3-10TiO2/SBA-15784.820.826.19
    1.6WO3-15TiO2/SBA-15763.650.766.25
    1.6WO3-20TiO2/SBA-15683.420.656.23
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  • 收稿日期:  2015-10-28
  • 修回日期:  2015-12-16
  • 网络出版日期:  2021-01-23
  • 刊出日期:  2016-06-10

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