高等学校化学学报 ›› 2002, Vol. 23 ›› Issue (4): 656.

• 研究论文 • 上一篇    下一篇

含钴、锰杂原子分子筛上烷烃低温分子氧氧化

田鹏, 许磊, 黄韬, 谢鹏, 刘中民   

  1. 中国科学院大连化学物理研究所, 大连 116023
  • 收稿日期:2000-11-15 出版日期:2002-04-24 发布日期:2002-04-24
  • 通讯作者: 刘中民(1964年生),男,博士,研究员,博士生导师,从事分子筛合成、催化新材料的开发及应用、固体酸碱催化及其过程研究.E-mail:zml@ms.dicp.ac.cn E-mail:zml@ms.dicp.ac.cn

Alkane Oxidation on Co- and Mn-containing MolencularSieves by Molecular Oxygen

TIAN Peng, XU Lei, HUANG Tao, XIE Peng, LIU Zhong-Min   

  1. Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
  • Received:2000-11-15 Online:2002-04-24 Published:2002-04-24

摘要: 用水热法合成了MeAlPO-5,MeAPSO-35,MeAlPO-18(MeAPS-18(Me=Co,Mn)分子筛,并用XRD和TPD对其进行表征。考察了在氧气作氧化剂的情况下,辛烷在这些杂原子分子筛上的氧化反应行为。辛烷氧化反应产物中,除辛酮和辛醇外,还出现了辛烷裂解氧化产物和辛烷多氧代产物。不同结构的分子筛催化剂上,辛烷氧化反应产物的选择性差异不大。在含有较多酸中心的MeAPSO分子筛上,n(辛酮)/n(辛醇)比要高于相同结构的MeAlPO分子筛。催化剂转移实验显示,氧化反应在多相体系中进行。考察了反应时间和温度变化对辛烷氧化反应的转化率及产物选择性等的影响,根据实验结果对反应机理进行了讨论。

关键词: 杂原子分子筛, 氧气, 烷烃, 氧化

Abstract: MeAlPO-5, MeAPSO-35, MeAlPO-l8 and MeAPSO-18(Me=Co, Mn) were prepared by hy-drothermal synthesis and were characterized by XRDand TPD(NH3).Their catalytic properties for theoxidation of octane were studied by using oxygen as the oxidant.In the oxidative products, there were oc-tanones, octanols, cracked oxygenates and oxygenates with more than one functional group.The selectivi-ty over different catalysts was similar.The ratio of n(octanone)/n(octanol) on MeAPSOwas higher thanthat over the same type MeAlPOmolecular sleve.The experiment of catalyst removal showed the oxida-tion was a heterogeneous reaction.Moreover, the effects of reaction time and temperature on the oxidationwere also investigated.According to the results, we discussed the reaction mechanism.

Key words: Molecular sieves containing metals, Oxygen, Alkane, Oxidation

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