【作者】 姜红石；

【导师】 钟邦克；

【作者基本信息】 暨南大学 ， 无机化学， 2000， 硕士

【摘要】 丙烯酸是重要的有机化工原料。丙烷选择氧化制丙烯酸是有效利用丙烷的重要途径，相对丙烯氧化制丙烯酸而言，其原料来源更廉价丰富，具有潜在的工业应用前景。 杂多化合物是目前少有的优良多功能催化剂，近年来用杂多化合物选择催化氧化丙烷已成为研究热点。但这些研究大多是从组成和结构方面进行改进。 本文着重从价态考虑，改进了制备方法，使杂多化合物部分还原，将还原型杂多化合物用于丙烷的选择氧化反应。经过一系列的评价筛选，发现用Cu粉制得的还原型杂多化合物，以浸渍法载荷在经水热扩孔的载体SiO₂上，并在还原性气氛下反应时，取得较好的效果。得到最佳催化剂的组成为：杂多化合物—Cu_0.6Cr_0.6PAs_0.6Mo₁₀V₂O_x；载体—SiO₂（220℃扩孔）。 对工艺条件进行了研究，探讨了温度、空速、原料比、水的引入等对催化活性的影响，得到最佳反应条件为：温度—390℃；空速—1500h^-1；反应气组成—C₃H₈∶O₂∶N₂∶H₂O=2∶1∶5∶2（mol/mol）。在此条件下，丙烷转化率为38％，丙烯酸收率达14.8％。 同时采用IR，DTA，SEM，ESR，孔径及比表面测定等对催化剂进行了一系列的表征。更多还原

【Abstract】 Acrylic Acid (AA) is a very important raw material in organic chemical industry. Selective oxidation of propane to produce AA is an important way to use propane effectively. Compared with the oxidation of propene to produce AA, the material of this way is very rich and inexpensive. It has a potential foreground of industrial applications.Heteropoly compound (HPC) is a kind of excellent versatile catalyst. Using HPC catalyst to oxide selectively propane has become very popular recently. However, most of these studies just focused on the constituent and structure to improve the catalytic activity.This work placed stress on the state of valence, changing the preparation method to prepare partial reduced HPC, and using the partial reduced HPC as catalyst creatively to selective oxidation of propane.The systematic research was proceeded on the HPC and the carriers. It was found that the catalytic activity of the HPC which was prepared from Cu powder, being carried on Si02 (whose pore has been expanded by heat water steam in high-pressure container) as catalyst and in reduced air (fuel-rich condition), is very high. The optimum catalyst is: HPC?Cuo.oCro.6PAso.6MoioV2O~ carrier?Si02 (220 0C).The reaction techniques of selective catalytic oxidation of propane were evaluated. The influences of the reaction temperature, the total space velocity and the content of propane, oxygen, steam, were concerned. The optimum reaction conditions were chosen as following: reaction temperature?900C; total space velocity 500 W? the content of reaction gas?C3H8:02:N2:H20 2:l:5:2 (mol / mol); Under forementioned condition, the conversion of propane is 38%, the yield of AA reached14.8%.A series of characterization of catalysts were carried out, including IR, DTA, SEM, ESR etc.更多还原