【作者】 刘春丽；

【导师】 薛建伟；

【作者基本信息】 太原理工大学 ， 应用化学， 2008， 硕士

【摘要】 本文研究了杂多酸复合物的制备以及将其用于催化环己酮的自缩合反应生成2-（1-环己烯基）环己酮。课题采用了两种典型方法即回流吸附法、浸渍法制备杂多酸复合物。通过X射线衍射、热分析、红外光谱等手段对制备的杂多酸复合物进行了表征。考察得到了这一催化反应过程中的最佳工艺条件及催化剂的寿命。首先,选用活性炭为载体采用回流吸附法负载磷钨酸制备复合物(PW₁₂/C)。通过差热分析表明复合物中磷钨酸的分解逐步发生,红外谱图表明活性炭上Keggin结构的磷钨酸分解温度在600℃附近。PW₁₂/C用于催化合成2-（1-环己烯基）环己酮,实验得到最佳工艺条件:复合物中磷钨酸的负载量25%催化效果最佳,用量占反应物质量的3.0%,反应时间2.5h,反应温度150℃。其次,SBA-15分子筛具有高的比表面积,长程有序的孔道等特点,是良好的催化剂载体。SBA-15分子筛本身不具有酸性,本文采用浸渍法在该分子筛上引入磷钨酸,使其具有一定的酸强度。采用浸渍法将磷钨酸负载到SBA-15分子筛内制备复合物(PW₁₂/SBA-15)。磷钨酸均匀分散于SBA-15分子筛内,保持Keggin结构不变。复合物中SBA-15载体与磷钨酸有较强的相互作用,造成载体的水热稳定性下降及磷钨酸的热稳定性下降。最后,将磷钨酸、磷钼酸按一定比例进行复配,采用浸渍法制备成负载型催化剂,催化合成2-（1-环己烯基）环己酮催化效果好,转化率达到86.5%,具有很好的工业应用前景。更多还原

【Abstract】 In this work, we studied preparation of 12-tungstophosphoric acid composites, and then composites were employed as catalysts to synthesize 2-（1-cyclohexenyl）cyclohexanone in this paper. A series of 12-tungstophosphoric acid composites were prepared by two typical methods, namely reflux adsorption method and impregnation method. The composites were characterized by XRD,TG-DTA, IR etc. The optimum reaction conditions and longevity of catalysts were investigate.First of all, active carbons were selected as supports to prepare 12-tungstophosphoric acid composites （PW12/C） by reflux adsorption method. The results of TG-DTA and other different analysis indicated that 12-tungstophosphoric acids decomposed gradually through analysis of samples calcined composites under the different temperatures. From the infrared spectrometry, we known the Keggin structure of 12-tungstophosphoric acid decomposed at the 600℃. The PW₁₂/C were used as catalysts for the synthesis of 2-（1-cyclohexenyl）cyclohexanone. The optimum reaction conditions were as follows:amount of 12-tungstophosphoric acid supported on active carbon 25%, amount of the catalyst used in the reactants 3.0%, reaction time 2.5h, reaction temperature 150℃.Secondly, The molecular sieve SBA-15 has more good characters, such as higher specific surface, uniform porous channels. It is regarded as an excellent support. The molecular sieve SBA-15 itself does not has acidity. In this paper 12-tungstophosphoric acids were introduced in the mesoporous molecular sieve by impregnation method. The 12-tungstophosphoric acids also highly dispersed in the molecular sieve and kept Keggin structure. In the composites there are strong mutual interaction between the support SBA-15 and 12-tungstophosphoric acid, the hydrothermal stability of support and acid all dropped.Finally, Phosphotungstic acid and phosphomolybdic acid were mixed in 1:1 proportion, The Catalytic activity was good when it was supported by Impregnation method, During the synthesis of 2-（1-cyclohexenyl）cyclohexanone, Conversion of cyclohexanone could reach 86.5%,The catalyst had favorable Industrial prospect.更多还原