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Pt掺杂Ni/NiAlOx催化菲加氢饱和反应性能研究

刘道诚 荆洁颖 王九占 冯杰 李文英

刘道诚, 荆洁颖, 王九占, 冯杰, 李文英. Pt掺杂Ni/NiAlOx催化菲加氢饱和反应性能研究[J]. 燃料化学学报. doi: 10.1016/S1872-5813(21)60128-7
引用本文: 刘道诚, 荆洁颖, 王九占, 冯杰, 李文英. Pt掺杂Ni/NiAlOx催化菲加氢饱和反应性能研究[J]. 燃料化学学报. doi: 10.1016/S1872-5813(21)60128-7
LIU Dao-cheng, JING Jie-ying, WANG Jiu-zhan, FENG Jie, LI Wen-ying. Performance of Pt-doped Ni/NiAlOx catalysts for phenanthrene hydrogenation saturation[J]. Journal of Fuel Chemistry and Technology. doi: 10.1016/S1872-5813(21)60128-7
Citation: LIU Dao-cheng, JING Jie-ying, WANG Jiu-zhan, FENG Jie, LI Wen-ying. Performance of Pt-doped Ni/NiAlOx catalysts for phenanthrene hydrogenation saturation[J]. Journal of Fuel Chemistry and Technology. doi: 10.1016/S1872-5813(21)60128-7

Pt掺杂Ni/NiAlOx催化菲加氢饱和反应性能研究

doi: 10.1016/S1872-5813(21)60128-7
基金项目: 国家自然科学基金资助项目(21978190,22038008)
详细信息
    作者简介:

    刘道诚(1996-),男,硕士研究生,化学工程专业,研究方向为煤基粗油加氢提质

    通讯作者:

    Tel/Fax:86-351-6018453. E-mail:jingjieying@tyut.edu.cn(荆洁颖)

    ying@tyut.edu.cn(李文英)

  • 中图分类号: TQ426

Performance of Pt-doped Ni/NiAlOx catalysts for phenanthrene hydrogenation saturation

Funds: The project was supported by National Natural Science Foundation of China (21978190, 22038008)
  • 摘要: 受空间位阻的影响,末环的吸附活化是稠环芳烃加氢饱和反应的难点之一。本文选取菲为模型化合物,以强化芳烃吸附为目标,采用等体积浸渍法制备了系列Pt-Ni/NiAlOx催化剂,系统考察了Pt掺杂量对催化剂结构和菲加氢饱和性能的影响。结果表明:当反应温度300 ℃、氢气压力5 MPa、重时空速52 h−1时,相比Ni/NiAlOx催化剂,掺杂0.5 wt%Pt的0.5Pt-Ni/NiAlOx催化剂上全氢菲选择性在反应8 h后由40%提升至67%,且表观反应速率和转化频率分别由1.53 × 10−3 mol/kg/s和14.64 × 10−3 s−1提升至1.81 × 10−3 mol/kg/s/和22.16 × 10−3 s−1。这主要归因于金属Pt适宜的掺杂量提高了金属Ni缺电子结构的稳定性,促进芳烃吸附,提升了菲加氢饱和性能。
  • 图  1  不同Pt负载量的催化剂(a)焙烧后与(b)还原后XRD图谱

    Figure  1  XRD spectra of catalysts after calcination (a) and reduction (b) with different Pt loadings

    图  2  不同Pt负载量的Pt-Ni/NiAlOx催化剂H2-TPR图谱

    Figure  2  H2-TPR spectra of Pt-Ni/NiAlOx catalysts with different Pt loadings

    图  3  不同Pt负载量的Pt-Ni/NiAlOx催化剂Ni 2p轨道XPS谱图

    Figure  3  XPS spectra in the Ni 2p region of the Pt-Ni/NiAlOx catalysts with different Pt loadings

    图  4  不同Pt负载量Pt-Ni/NiAlOx催化剂活性评价

    Figure  4  The selectivity of perhydrophenanthrene over Pt-Ni/NiAlOx catalysts with different Pt loadings

    图  5  不同Pt负载量的催化剂反应后XRD图谱

    Figure  5  XRD spectra of catalysts after reaction with different Pt loadings

    图  6  不同负载量Pt-Ni/NiAlOx催化剂菲加氢反应后的Ni 2p轨道XPS谱图

    Figure  6  XPS spectra in the Ni 2p region of the Pt-Ni/NiAlOx catalysts with different Pt loadings after PHE hydrogenation

    图  7  (a)还原后0.25Pt-Ni/NiAlOx、(b)还原后0.5Pt-Ni/NiAlOx、(c)还原后0.75Pt-Ni/NiAlOx催化剂以及(d)反应后0.5Pt-Ni/NiAlOx催化剂TEM图

    Figure  7  TEM images of (a) fresh 0.25Pt-Ni/NiAlOx, (b) fresh 0.5Pt-Ni/NiAlOx, (c) fresh 0.75Pt-Ni/NiAlOx catalysts and (d) spent 0.5Pt-Ni/NiAlOx catalysts

    表  1  不同Pt负载量的Pt-Ni/NiAlOX催化剂比表面积和平均孔径

    Table  1  The surface area and average pore size of Pt-Ni/NiAlOX catalysts with different Pt loadings

    Catalyst$ {\rm{S}}_{{\rm{BET}}}^{\rm{a}}$/ m2·g−1$ {\rm{S}}_{{\rm{meso }}}^{\rm{b}}$/ m2·g−1$ {\rm{S}}_{{\rm{mic}}}^{\rm{b}}$/ m2·g−1Average pore size/ nm
    0.25Pt-Ni/NiAlOX177.5177.5-5.2
    0.5Pt-Ni/NiAlOX163.4163.4-4.4
    0.75Pt-Ni/NiAlOX162.1162.1-4.8
    Ni/NiAlOX178.0178.0-4.5
    a: BET surface area. b: Calculated by t-plot. All of the samples are tableted at 15 MPa
    下载: 导出CSV

    表  2  系列Pt-Ni/NiAlOX催化剂金属分散度及本征动力学

    Table  2  Metal dispersion and intrinsic activity of Pt-Ni/NiAlOX catalysts with different Pt loadings

    CatalystMetal dispersiona/ %Hydrogenation conversion of PHE / %robs × 103 / mol·g−1s−1TOF × 103 / s−1Ref.
    0.25Pt-Ni/NiAlOX0.9410.91 b1.2018.68 bThis work
    0.5Pt-Ni/NiAlOX1.1415.68 b1.8122.16 bThis work
    0.75Pt-Ni/NiAlOX1.7614.31 b1.6313.48 bThis work
    Ni/NiAlOX1.9918.50 c1.5314.64 cThis work
    0.5Pt/Al2O399.126.24 d0.050.58 dThis work
    NiMoS/MZSM-5//0.741.80[26]
    Ni2P/HZSM-5-M//1.328.20[27]
    a: Calculated by CO pulse adsorption. b: Determined at 300 ℃, H2 pressure of 5 MPa, 1 wt% PHE in decalin, WHSV of 720 h−1. c: Determined at 300 ℃, H2 pressure of 5 MPa, 1 wt% PHE in decalin, WHSV of 520 h−1. d: Determined at 300 ℃, H2 pressure of 5 MPa, 1 wt% PHE in decalin, WHSV of 52 h−1
    下载: 导出CSV
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  • 收稿日期:  2021-05-08
  • 修回日期:  2021-06-15
  • 网络出版日期:  2021-07-16

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