Pt掺杂Ni/NiAlOx催化菲加氢饱和反应性能研究

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

  • 摘要: 本研究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%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−1·s−1和14.64 × 10−3 s−1提升至1.81 × 10−3 mol·kg−1·s−1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。

     

    Abstract: Limited by the steric hindrance, hydrogenation of the final unsaturated ring in polycyclic aromatic hydrocarbons remains a challenge. In this work, a series of Pt-Ni/NiAlOx catalysts were synthesized by impregnation method to enhance the adsorption of aromatics, and phenanthrene was served as the model compound. The effects of Pt content on the structure and saturation performance of Pt-Ni/NiAlOx catalysts were systematically investigated. When the saturation reaction was performed at 300 ℃, 5 MPa and a weight hourly space velocity of 52 h−1, the selectivity of perhydrophenanthrene could be enhanced from 40% over Ni/NiAlOx catalysts to 67% over 0.5Pt-Ni/NiAlOx catalysts with 0.5% Pt loading. Meanwhile, the obvious reaction rate and turnover frequency were also improved from 1.53×10−3 mol·kg−1·s−1 and 14.64×10−3 s−1 to 1.81×10−3 mol·kg−1·s−1 and 22.16×10−3 s−1 respectively. This is related to the modified stability of metallic electron-deficient structure of Ni by Pt introduction in phenanthrene hydrogenation, which can promote the adsorption of aromatic hydrocarbons as well as the hydrogenation activity.

     

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