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动态法晶化合成钛硅分子筛及其脱硫性能研究

唐明宇 王海彦 任铁强 魏民 孙娜 先宏飞

唐明宇, 王海彦, 任铁强, 魏民, 孙娜, 先宏飞. 动态法晶化合成钛硅分子筛及其脱硫性能研究[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2021054
引用本文: 唐明宇, 王海彦, 任铁强, 魏民, 孙娜, 先宏飞. 动态法晶化合成钛硅分子筛及其脱硫性能研究[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2021054
TANG Ming-yu, WANG Hai-yan, REN Tie-qiang, WEI Min, SUN Na, XIAN Hong-fei. Preparation of TS-1 by dynamic method and study on the performance of thiophene sulfur removal[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2021054
Citation: TANG Ming-yu, WANG Hai-yan, REN Tie-qiang, WEI Min, SUN Na, XIAN Hong-fei. Preparation of TS-1 by dynamic method and study on the performance of thiophene sulfur removal[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2021054

动态法晶化合成钛硅分子筛及其脱硫性能研究

doi: 10.19906/j.cnki.JFCT.2021054
基金项目: 国家自然科学基金(2017LQN006)和辽宁省教育厅科研项目(L2019014)资助
详细信息
    作者简介:

    唐明宇:yytmy091928@163.com

    通讯作者:

    E-mail:fswhy@126.com

  • 中图分类号: TQ426.6

Preparation of TS-1 by dynamic method and study on the performance of thiophene sulfur removal

Funds: The project was supported by the National Natural Science Foundation of China (2017LQN006) and the Education Department of Liaoning Province (L2019014)
  • 摘要: 本研究以四丙基氢氧化铵(TPAOH)为模板剂,正硅酸乙酯(TEOS)为硅源,钛酸四丁酯(TBOT)为钛源,在动态晶化釜内合成形貌规则且粒径约为600 nm的TS-1分子筛。通过改变TBOT的用量,进而改变初始合成液中的硅钛比,考察硅钛比对TS-1分子筛的影响,并采用SEM、TEM、XRD、FT-IR、UV-vis、XPS、N2吸附-脱附技术对制得的催化剂进行表征。将合成得到的TS-1分子筛应用于以噻吩正辛烷为模拟油的体系中,考察TS-1分子筛催化氧化脱硫性能。
  • 图  1  不同方式制备TS-1分子筛的XRD、紫外可见光谱谱图

    Figure  1  XRD patterns, UV-vis spectra of TS-1 samples prepared in different ways

    图  2  不同硅钛比TS-1样品的XRD谱图

    Figure  2  XRD patterns of TS-1 samples with different ratios of silicon to titanium

    图  3  不同硅钛比TS-1样品的SEM照片

    (a): TS-1(20); (b): TS-1(30); (c): TS-1(40)

    Figure  3  SEM images of TS-1 samples with different ratios of silicon to titanium

    图  4  TS-1(30)样品的TEM照片

    Figure  4  TEM images of TS-1(30) sample

    图  5  不同硅钛比TS-1的傅里叶变换红外光谱谱图

    Figure  5  FT-IR spectra of TS-1 samples with different ratios of silicon to titanium

    图  6  不同硅钛比TS-1样品的紫外可见光谱谱图

    Figure  6  UV-vis spectra of TS-1 samples with different ratios of silicon to titanium

    图  7  不同硅钛比TS-1样品的氮气吸附-脱附等温线

    Figure  7  Relative pressure N2 adsorption-desorption isotherms of TS-1 samples with different ratios of silicon to titanium

    图  8  不同硅钛比TS-1样品的 DFT孔径分布

    Figure  8  DFT pore size distributions of TS-1 samples with different ratios of silicon to titanium

    图  9  不同硅钛比TS-1样品的 XPS谱图

    Figure  9  XPS spectra of TS-1 samples with different ratios of silicon to titanium

    图  10  不同硅钛比TS-1样品在H2O2中催化氧化噻吩

    Figure  10  Catalytic oxidation of thiophene (Th) with H2O2 over TS-1 samples with different ratios of silicon to titanium

    表  1  合成TS-1分子筛初始合成液组成

    Table  1  Initial gel composition of TS-1 synthesis

    SampleInitial gel composition
    TS-1(20)1.0SiO2∶0.050TiO2∶0.3TPAOH∶50H2O
    TS-1(30)1.0SiO2∶0.033TiO2∶0.3TPAOH∶50H2O
    TS-1(40)1.0SiO2∶0.025TiO2∶0.3TPAOH∶50H2O
    下载: 导出CSV

    表  2  不同硅钛比TS-1体相的元素原子百分比

    Table  2  Elements atomic percentage of overall TS-1 samples with different ratios of silicon to titanium

    SampleElement atomic percentage/%
    TS-1(20)62.5236.780.69
    TS-1(30)60.0139.260.73
    TS-1(40)60.5838.950.47
    下载: 导出CSV

    表  3  不同硅钛比TS-1的孔结构性质

    Table  3  Pore structure properties of TS-1 samples with different ratios of silicon to titanium

    SampleSt/
    (m2·g−1
    Sm/
    (m2·g−1
    dp/
    nm
    vm/
    (cm3·g−1
    vt/
    (cm3·g−1
    TS-1(20)512.4483.62.1540.210.28
    TS-1(30)513.9483.42.2750.210.29
    TS-1(40)464.0418.62.1680.180.25
    下载: 导出CSV

    表  4  不同物质光电能谱峰处结合能

    Table  4  Binding energy of different samples

    SampleTi 2p3/2 E/eV
    αβ
    TS-1460.0 ± 0.2457.9 ± 0.2
    TiO2 + SiO2458.0
    TiO2458.8
    α represents the binding energy at the spectral peak of framework titanium; β represents the binding energy at the spectral peak of non-framework titanium (TiO2)
    下载: 导出CSV

    表  5  不同硅钛比TS-1表相的元素原子百分比

    Table  5  Elements atomic percentage of surface TS-1 samples with different ratios of silicon to titanium

    SampleElement atomic percentage/%
    TS-1(20)60.1729.910.68
    TS-1(30)59.4229.900.68
    TS-1(40)59.5130.460.29
    下载: 导出CSV
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  • 收稿日期:  2021-03-04
  • 修回日期:  2021-05-07
  • 网络出版日期:  2021-06-04

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