Abstract:

Catalytic hydrodenitrogenation under mild conditions was improved by using modified solid catalyst coupled with[Bmim]BF₄ ionic liquid.Ni₂P/SBA-15 catalyst was modified with different Mo loadings and structures of Mo-Ni₂P/SBA-15 modified catalysts were characterized by N₂ adsorption-desorption,X-ray diffraction,and X-ray photoelectron spectroscopy.These catalysts coupled with[Bmim]BF₄ were evaluated for denitrification of pyrrolidine model compound in batch reactor at mild pressure and temperature.The results showed that Mo addition improved catalytic hydrodenitrogenation activity.At low temperature,the denitrification process was dominated by ionic liquid extraction.As temperature was increased,coupling hydrodenitrogenation was more obvious.5% Mo-25% Ni₂P/SBA-15 catalyst coupled with[Bmim]BF₄ exhibited the best hydrodenitrogenation efficiency up to 80.1% at 150℃ and 3 MPa.Furthermore,the ionic liquid did not show significant decrease in hydrogenation efficiency after four cycles.The presence of ionic liquids achieved good catalytic hydrodenitrogenation under mild conditions,which could be a new process for catalytic hydrogenation under low temperature and pressure conditions.

Key words: ionic liquid, coupling, catalyst, hydrogenation, extraction, denitrification, mild

摘要：

通过改性固体催化剂，耦合离子液体进行催化反应，实现了在温和条件下催化加氢脱氮性能的提高。采用助剂Mo对Ni₂P/SBA-15催化剂进行改性，并用XRD、BET、XPS对催化剂结构进行表征。以吡啶为含氮模型化合物，将固体催化剂耦合[Bmim]BF₄在温和的条件下进行加氢脱氮活性评价。结果表明，低温时的脱氮过程主要以离子液体萃取为主；随着温度的升高，耦合加氢脱氮效果表现显著，且改性后的5% Mo-25% Ni₂P/SBA-15催化剂耦合离子液体在150℃、3 MPa的条件下评价脱氮率最高，达到了80.1%。离子液体4次加氢循环之后，其加氢性能没有明显的下降。离子液体的参与使得催化加氢脱氮反应在温和的条件下得以实现，这为催化加氢在低温低压条件下提供了新的理论和工艺。

关键词: 离子液体, 耦合, 催化剂, 加氢, 萃取, 脱氮, 温和