中华医学超声杂志

应用化学 ›› 2011, Vol. 28 ›› Issue (02): 188-193.DOI: 10.3724/SP.J.1095.2011.00260

• 研究论文 • 上一篇    下一篇

Co-MCM-41催化H2O2氧化4-甲基吡啶生成4-吡啶甲酸的反应条件及机理

缪应纯1*,翟忠标2,杨盛春3,王家强3   

  1. (1.曲靖师范学院化学化工学院 曲靖 655011；2.昆明冶金研究院 昆明；3.云南大学应用化学系 昆明)
  • 收稿日期:2010-05-05 修回日期:2010-07-24 出版日期:2011-02-10 发布日期:2011-02-10
  • 通讯作者: 缪应纯，讲师; E-mail:miaoyingchun1979@126.com; 办公电话：0874-8998658; 研究方向：催化剂制备、光催化和催化氧化
  • 基金资助:
    云南省教育厅科学研究基金(09Y0392)曲靖师范学院科学研究基金(2009QN032)曲靖师范学院应用电化学及材料制备研究创新团队(TD200901)曲靖师范学院资源与环境化学重点实验室资助项目

Catalytic Oxidation of 4-Methyl Pyridine to Isonicotinic Acid by H2O2 over Co-MCM-41

MIAO Ying-Chun1*, ZHAI Zhong-Biao2, YANG Sheng-Chun3, WANG Jia-Qiang3   

  1. (1.Department of Chemistry and Chemical Engineering,Qujing Normal University,Qujing 655000;
    2.Kunming Metallurgy Research Institute,Kunming;
    3.Department of Applied Chemistry,Yunnan University,Kunming)
  • Received:2010-05-05 Revised:2010-07-24 Published:2011-02-10 Online:2011-02-10

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摘要：

研究了乙酸溶剂中无引发剂条件下，Co掺杂MCM-41催化过氧化氢（30%）氧化4-甲基吡啶的反应，催化剂表现出高底物转化率和产物吡啶甲酸选择性以及良好的再生性。 探讨了不同溶剂、反应时间、反应温度、催化剂用量等对H2O2氧化4-甲基吡啶反应的影响，确定较优反应条件为m（4-甲基吡啶)∶m（催化剂)=10∶1，V（4-甲基吡啶)∶V（冰醋酸)=1∶10，温度363 K，时间6 h。 该条件下4-甲基吡啶的转化率为96.5%，4-吡啶甲酸的选择性为91.4%。 探讨了可能的反应机理。

关键词: 介孔材料, 催化氧化, 甲基吡啶, 吡啶甲酸

Abstract:

Liquid phase oxidation of 4-methylpyridine(4-MP) was carried out under mild reaction conditions over mesoporous Co-MCM-41 catalysts using aqueous hydrogen peroxide(30%) as oxidant and acetic acid as solvent without adding any initiator. The catalysts exhibited high substrate conversion and good product isonicotinic acid(4-PCA) selectivity. Recycling of the catalyst indicates that the catalyst can be used for a number of times without losing its activity significantly. The effects of solvent, reaction time, catalyst concentration, and reaction temperature on the catalyst performance were examined in order to optimize the conversion of 4-methylpyridine and the selectivity of isonicotinic acid. A 91.4% selectivity to isonicotinic acid was obtained at 96.5% conversion of 4-methylpyridine under the optimum reaction conditions:m(4-methyl pyridine)∶m(catalyst)=10∶1, V(4-methyl pyridine)∶V(acetic acid glacial)=1∶10, reaction temperature=363 K, reaction time=6 h. The reaction mechanism is proposed based on the results.

Key words: Co-MCM-41, catalytic oxidation, methyl pyridine, isonicotinic acid

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