Solid-Phase Synthesis of Nickel-Molybdenum Catalysts for Metathesis of Propylene under Mechanical Action

O. A. Knyazheva, O. N. Baklanova, E. A. Buluchevskiy, A. Arbuzov, M. V. Trenikhin, Т. Р. Karpova, M. Moiseenko, N. N. Leontieva, A. V. Lavrenov
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Abstract

The solid-phase synthesis of model aluminum-molybdenum (Al-Mo) and aluminum-nickel-molybdenum (Al-Ni-Mo) compositions constituting the catalysts for metathesis of propylene was carried out under mechanical action. The structure of model Al-Mo and Al-Ni-Mo compositions was studied using X-ray diffraction analysis, high-resolution transmission electron microscopy, infrared spectroscopy, and diffuse reflectance electron spectroscopy (UV-vis DRS). The latter method revealed the presence of isolated monomeric and oligomeric molybdate compounds in the model Al-Ni-Mo compositions. Granulated catalysts for metathesis were obtained by molding the model Al-Mo and Al-Ni-Mo compositions with aluminum hydroxide followed by calcination. Most active in the metathesis of propylene was the aluminum-molybdenum catalyst containing 2.6 wt.% Ni, 13.0 wt.% Mo and 32.7 wt.% Al. At the process temperature of 200 °С, pressure 0.1 MPa, and weight space velocity of propylene 1 h–1, the conversion of propylene on this catalyst reached 33.7 %, which makes the catalyst promising for practical application. Therewith, the weight fraction of ethylene in the reaction products was 17.5 %, and butenes – 71.3 %.
机械作用下丙烯还原反应镍钼催化剂的固相合成
在机械作用下,固相合成了模型铝钼(Al-Mo)和铝镍钼(Al-Ni-Mo)组成的丙烯复分解催化剂。利用x射线衍射分析、高分辨率透射电镜、红外光谱和漫反射电子能谱(UV-vis DRS)研究了模型Al-Mo和Al-Ni-Mo成分的结构。后一种方法揭示了在模型Al-Ni-Mo组合物中存在分离的单体和低聚钼酸盐化合物。用氢氧化铝对模型Al-Mo和Al-Ni-Mo组分进行模塑,然后煅烧,得到了颗粒状的复分解催化剂。其中,Ni含量为2.6 wt.%、Mo含量为13.0 wt.%、Al含量为32.7 wt.%的铝钼催化剂反应最活跃。在工艺温度为200°С、压力为0.1 MPa、丙烯质量空速为1 h-1的条件下,丙烯的转化率可达33.7%,具有较好的实际应用前景。由此,反应产物中乙烯的质量分数为17.5%,丁烯的质量分数为- 71.3%。
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