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The effect of surface acidic and basic properties on the hydrogenation of aromatic rings over the supported nickel catalysts

机译:表面酸性和碱性对负载型镍催化剂上芳环加氢的影响

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Ni/Al2O3, Ni/MgAlO and Ni/MgO catalysts containing about 60 wt% of nickel were prepared by the co-precipitation method. The textural and structural properties were characterized and it was found that the dispersion of nickel was high in these catalysts. The active nickel surface area was found to be high (78 m~2/gcat.) in Ni/MgAlO, corresponding to the average nickel particle size of 3.5 nm. Microcalorimetric adsorption of NH3 and CO2 showed that the Ni/Al2O3 and Ni/MgO exhibited strong surface acidity and basicity, respectively, while the Ni/MgAlO possessed both surface acidity and basicity. In addition, both the initial heat and coverage were higher on Ni/Al2O3 than on Ni/MgO for the adsorption of toluene, indicating the strong interaction between the aromatic rings in toluene (that may act as a Lewis base due to the enriched electron densities) and the surface acidic sites on the support. The adsorption of toluene on the metallic nickel surface produced higher heat, indicating the strong interaction of the π electrons in aromatic rings of toluene with the d orbitals of surface nickel atoms. Although the adsorption of H2 showed the higher active surface nickel area in Ni/MgAlO than in Ni/Al2O3, the activities of hydrogenation of toluene and phenol were significantly higher on Ni/Al2O3 than on Ni/MgAlO, indicating the important effect of surface acidity on the hydrogenation of aromatic rings.
机译:通过共沉淀法制备了含有约60重量%镍的Ni / Al 2 O 3,Ni / MgAlO和Ni / MgO催化剂。表征了结构和结构性质,发现在这些催化剂中镍的分散度高。发现镍/ MgAlO中的活性镍表面积很高(78 m〜2 / gcat。),对应于3.5 nm的平均镍粒度。 NH3和CO2的微量热吸附表明,Ni / Al2O3和Ni / MgO分别具有很强的表面酸性和碱性,而Ni / MgAlO兼具表面酸性和碱性。此外,对于甲苯吸附,Ni / Al2O3的初始热量和覆盖率均高于Ni / MgO,这表明甲苯中的芳环之间有很强的相互作用(由于富电子密度,它可能充当路易斯碱) )和载体上的表面酸性部位。甲苯在金属镍表面上的吸附会产生更高的热量,表明甲苯芳环中的π电子与表面镍原子的d轨道之间存在较强的相互作用。尽管H2的吸附显示Ni / MgAlO中的活性表面镍面积比Ni / Al2O3中的高,但甲苯和苯酚的氢化活性在Ni / Al2O3上明显高于在Ni / MgAlO上,表明表面酸度的重要影响芳环的氢化。

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