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化学学报
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化学学报 ›› 2010, Vol. 68 ›› Issue (21): 2145-2150.    下一篇

研究论文

Nafion功能化介孔催化剂上苯甲醚/苯甲酰氯酰基化反应研究

顾怡1，匡伟伟2，徐源吉1，徐华龙1，沈伟*,1   

  1. (1上海市分子催化和功能材料重点实验室 先进材料实验室 复旦大学化学系 上海 200433)
    (2上海华谊集团上硫化工有限公司 上海 200431)
  • 投稿日期:2010-05-15 修回日期:2010-06-12 发布日期:2010-07-14
  • 通讯作者: 沈伟 E-mail:wshen@fudan.edu.cn
  • 基金资助:

    863重点计划;上海市科学技术委员会基金

Catalytic Acylation of Anisole and Benzoyl Chloride over Nafion Functionalized Mesoporous Catalysts

Gu Yi1 Kuang Weiwei2 Xu Yuanji1 Xu Hualong1 Shen Wei*,1   

  1. (1 Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Laboratory of Advanced Materials, Department of Chemistry, Fudan University, Shanghai 200433)
    (2 Shanghai Huayi Group Shanghai Shangliu Chemical Co., LTD, Shanghai 200431)
  • Received:2010-05-15 Revised:2010-06-12 Published:2010-07-14
  • Contact: Wei Shen E-mail:wshen@fudan.edu.cn

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1144

被引次数

7

苯甲醚/苯甲酰氯的酰基化产物4-甲氧基二苯甲酮是多种精细化工产品的重要中间体. 本工作主要介绍了Nafion负载型SBA-15, SBA-16及Me-SBA-15介孔超强酸催化剂的制备及其在苯甲醚/苯甲酰氯酰基化反应中的应用. 实验结果表明, 单位时间单位Nafion活性位上的苯甲酰氯转化数高于传统HBeta沸石和硫酸氧化锆, 且载量的增加能显著提高酰基化催化性能. 甲基修饰的Me-SBA-15介孔材料明显改善了催化剂表面的疏水性能, 有效减缓了多聚芳烃副产物的生成, 反应的转化率得到大幅提高. 相对一维孔道结构的介孔SBA-15而言, 三维笼状结构的SBA-16对反应物及产物分子具有更好的扩散性能, 该结构优势由酰基化反应的高初始活性得以充分体现. 在整个反应过程中, 该类催化剂对4-甲氧基二苯甲酮具有专一的选择性.

关键词: Nafion树脂, 疏水表面, SBA-15, SBA-16, 苯甲醚/苯甲酰氯酰基化反应

Acylation reaction of anisole and benzoyl chloride produces 4-methoxybenzophenone which is an important intermediate for producing fine chemicals. In this work, Nafion impregnated SBA-15, SBA-16 and methyl-modified Me-SBA-15 catalysts were systematically synthesized and studied in this reaction. The results showed that the turnover frequencies over Nafion were higher than those over HBeta and sulfated zirconia and that the catalytic activity increased remarkably with the increasing of Nafion loading. The hydrophobicity modification of pore surface of SBA-15 promoted the conversion rate while reducing the polyaromatic byproducts. Nafion/SBA-16 is superior to Nafion/SBA-15 in molecular diffusion owning to its three-dimensional cubic structure, which was clearly shown in the initial activity. Selectivity of 4-methoxybenzophenone was favored during the reaction process.

Key words: Nafion resin, surface hydrophobicity control, SBA-15, SBA-16, acylation reaction of anisole and benzoyl chloride

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