物理化学学报 >> 2016, Vol. 32 >> Issue (12): 2961-2967.doi: 10.3866/PKU.WHXB201609181

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杂多酸/离子液体杂化材料催化苯的高选择性羟基化

马青1,2,童金辉1,2,*(),宿玲弟1,2,王文慧1,2,马文梅1,2,薄丽丽3   

  1. 1 西北师范大学化学化工学院,兰州730070
    2 生态环境相关高分子材料教育部重点实验室,兰州730070
    3 甘肃农业大学理学院,兰州730070
  • 收稿日期:2016-07-25 发布日期:2016-11-30
  • 通讯作者: 童金辉 E-mail:jinhuitong@126.com
  • 基金资助:
    国家自然科学基金;教育部长江学者和创新团队发展计划;和西北师范大学本科生学术能力提升计划项目资助

Highly Selective Hydroxylation of Benzene Catalyzed by Hybrids of Polyoxometalate/Ionic Liquid

Qing MA1,2,Jin-Hui TONG1,2,*(),Ling-Di SU1,2,Wen-Hui WANG1,2,Wen-Mei MA1,2,Li-Li BO3   

  1. 1 College of Chemistry and Chemical Engineering, Northwest Normal University, Lanzhou 730070, P. R. China
    2 Key Laboratory of Eco-Environment-Related Polymer Materials, Ministry of Education, Lanzhou 730070, P. R. China
    3 College of Science, Gansu Agricultural University, Lanzhou 730070, P. R. China
  • Received:2016-07-25 Published:2016-11-30
  • Contact: Jin-Hui TONG E-mail:jinhuitong@126.com
  • Supported by:
    国家自然科学基金;教育部长江学者和创新团队发展计划;和西北师范大学本科生学术能力提升计划项目资助

摘要:

制备了V取代的磷钼酸H3+xPMo12-xVxO40x=0,1,2)及1-丁基-3-甲基咪唑溴盐离子液体([C4mim]Br),并采用离子交换的方法制备了系列杂化材料([C4mim]3+xPMo12-xVxO40x=0,1,2);采用X射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)、紫外-可见漫反射光谱(UV-Vis DRS)对所制备样品进行了表征;以H2O2为氧化剂,考察了所得样品催化苯羟基化制苯酚的活性。结果表明,和相应的离子液体及杂多酸相比,杂化材料的催化活性得到了很大的提高,尤其是催化剂[C4mim]5PMo10V2O40,在优化后的条件下,苯的转化率可达到21%,苯酚的选择性在99%以上。而且,该催化剂具有很好的可重复使用性,连续使用五次后,苯的转化率和苯酚的选择性没有明显降低。

关键词: 杂多酸, 离子液体, 杂化材料, 苯羟基化

Abstract:

Aseriesof hybridmaterials ([C4mim]3+xPMo12-xVxO40, x=0, 1, 2)basedonV-substitutedphosphomolybdic acidH3+xPMo12-xVxO40 (x=0, 1, 2) and ionic liquid 1-butyl-3-methyl imidazolium bromide ([C4mim]Br) have been prepared by an anion-exchange method. The samples were characterized by X-ray diffraction (XRD), Fourier transform infrared spectrophotometry (FT-IR) and UV-Vis diffuse reflectance spectra (UV-Vis DRS) analysis. The catalytic performances of the samples were tested in oxidation of benzene to produce phenol using H2O2 as the oxidant. The results showed that the hybrids[C4mim]3+xPMo12-xVxO40 exhibit much higher catalytic properties than both the corresponding moieties. In particular, under the optimized conditions, 21% of benzene conversion and 99%selectivity for phenol have been obtained with[C4mim]5PMo10V2O40. The sample also exhibits good reusability and was reused five times without a significant decrease in conversion and selectivity.

Key words: Polyoxometalate, Ionic liquid, Hybrid material, Hydroxylation of benzene

MSC2000: 

  • O643