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分子氧存在下镁铝水滑石负载高锰酸钾活化醇类液相氧化反应研究
  • 期刊名称:高校化学工程学报, 22(4), 604-610, 2008
  • 时间:0
  • 分类:O643.32[理学—物理化学;理学—化学] TQ032.4[化学工程]
  • 作者机构:[1]茂名学院化工所,广东茂名525000, [2]南京信息工程大学环境科学与工程学院,江苏南京210044, [3]华南理工大学化学与化工学院,广东广州510640
  • 相关基金:国家自然科学基金(20576045)和新世纪优秀人才支持计划(NCET-06-740)资助.
  • 相关项目:界面聚合制备纳米金属盐和金属及其催化性能的研究
中文摘要:

用共沉淀和浸渍法分别制得镁铝水滑石固载MnO4^-催化剂HT-MnO4^-,并将该催化剂在温和条件下、以分子氧为氧化剂用于催化醇的液相氧化反应。以苯甲醇氧化反应为模型探讨了不同制备方法制得的催化剂以及温度、溶剂等条件对反应的影响,结果显示两种制备方法对催化性能影响的差别不大,非极性溶剂更有利于反应进行,苯甲醇转化牢随着温度上升明显提高。XRD表征给出水滑石经过MnO4^-阴离子交换以后,X射线衍射峰中最强峰对应晶面的平均粒径减小,但结构仍然完整;XPS表征表明HT-MnO4^-中Mn的结合能较之KMnO4中的Mn有所降低。说明镁铝水滑石负载高锰酸钾远比高锰酸钾温和,在醇的液相氧化中同时起着催化剂和氧化剂的作用。

英文摘要:

Mg-Al hydrotalcite-supported MnO4^- catalysts (HT-MnO4^-) were prepared separately by two different preparation methods (coprecipitation and impregnation methods), and their application to liquid-phase oxidation of alcohols in the present of molecular oxygen under mild condition was studied by using the oxidation of benzyl alcohol as the model alcohol oxidation reaction. It was found that the two HT-MnO4^- preparation methods exhibit only a few catalytic performance differences during alcohol oxidation reaction, while elevating reaction temperature and using non-polar solvent will favor the alcohol oxidation reaction. The XRD characterization of HT-MnO4^-shows that, since the anion MnO4^- substitutes the anion CO3^2- in the middle layer of hydrotalcite (HT), the average particle size of the crystal face corresponding to the most intensive X-ray diffraction peak decreases, while the structure of the HT remains unchanged. The XPS characterization indicates that the binding energy of Mn in HT-MnO4^- decreases in comparison with that in KMnO4. The oxidative performance of HT-MnO4^- is milder than that of KMnO4, and the Mg-Al hydrotalcite -supported MnO4^- catalyst plays dual roles of the catalyst and the oxidant in the alcohol oxidation reaction.

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