化工学报 ›› 2015, Vol. 66 ›› Issue (10): 3965-3970.DOI: 10.11949/j.issn.0438-1157.20150053

• 催化、动力学与反应器 • 上一篇    下一篇

Me-OMS-1s分子筛催化叔丁基过氧化氢分解制备叔丁醇

冯利利1, 卢书培2, 齐兴义2, 韩晓1   

  1. 1 北京建筑大学城市雨水系统与水环境教育部重点实验室, 北京市应对气候变化研究及人才培养基地, 北京 100044;
    2 北京航空航天大学化学与环境学院, 北京 100191
  • 收稿日期:2015-01-13 修回日期:2015-06-24 出版日期:2015-10-05 发布日期:2015-10-05
  • 通讯作者: 齐兴义
  • 基金资助:

    国家自然科学基金项目(51206009);北京市青年英才项目(YETP1663)。

Catalytic decomposition of tert-butyl hydroperoxide into tert-butyl alcohol over Me-OMS-1s molecular sieves

FENG Lili1, LU Shupei2, QI Xingyi2, HAN Xiao1   

  1. 1 Key Laboratory of Urban Stormwater System and Water Environment of Ministry of Education, Beijing Climate Change Response Research and Education Center, Beijing University of Civil Engineering and Architecture, Beijing 100044, China;
    2 School of Chemistry and Environment, Beihang University, Beijing 100191, China
  • Received:2015-01-13 Revised:2015-06-24 Online:2015-10-05 Published:2015-10-05
  • Supported by:

    supported by the National Natural Science Foundation of China (51206009) and the Beijing Higher Education Young Elite Teacher Project (YETP1663).

摘要:

采用静态水热法合成了Me-OMS-1s(Me=Mg,Co,Ni,Cu)分子筛催化剂,对合成的分子筛进行了X射线衍射和电感耦合等离子体发射光谱表征,并系统考察了反应温度(318~338 K)、反应时间(0.5~6 h)和催化剂用量(1.67~8.33 mg·ml-1)对Me-OMS-1s催化叔丁基过氧化氢分解制备叔丁醇反应性能的影响。研究结果表明,合成的分子筛均为钡镁锰矿型(todorokite)氧化锰;在选择的多相催化反应条件下,Me-OMS-1s均有催化叔丁基过氧化氢歧化分解的反应活性,反应物叔丁基过氧化氢具有较高的转化率,产物叔丁醇的选择性均为100%。Me-OMS-1s催化叔丁基过氧化氢歧化分解的反应活性顺序为:Cu-OMS-1 > Mg-OMS-1 > Ni-OMS-1 > Co-OMS-1。叔丁基过氧化氢的转化率随反应温度的升高、反应时间的延长和Me-OMS-1s用量的增大而显著增大。

关键词: 合成, Me-OMS-1s分子筛, 催化, 叔丁基过氧化氢, 制备, 叔丁醇

Abstract:

A series of Me-OMS-1s (Me=Mg, Co, Ni, Cu) molecular sieves was synthesized by the static hydrothermal method. The as-synthesized Me-OMS-1s were characterized by means of XRD and AES-ICP. The effects of reaction temperature (318—338 K), reaction time (0.5—6 h) and formal catalyst concentration (1.67—8.33 mg·ml-1) were investigated in detail on catalytic decomposition of tert-butyl hydroperoxide into tert-butyl alcohol over the as-synthesized Me-OMS-1s. The results showed that the synthetic Me-OMS-1s belonged to todorokite-type manganese oxides. All the Me-OMS-1 catalysts bore the activity for the catalytic disproportionation decomposition of tert-butyl hydroperoxide under the selected heterogeneous catalytic reaction conditions. The conversion of the reactant tert-butyl hydroperoxide under various reaction conditions was found to be high and the selectivity towards the product tert-butyl alcohol was 100%. The activity of Me-OMS-1s followed the order of: Cu-OMS-1 > Mg-OMS-1 > Ni-OMS-1 > Co-OMS-1. The conversion level of tert-butyl hydroperoxide was markedly enhanced with increasing reaction temperature, contact time and formal Me-OMS-1 concentration.

Key words: synthesis, Me-OMS-1s molecular sieves, catalysis, tert-butyl hydroperoxide, preparation, tert-butyl alcohol

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