含钴、锰杂原子分子筛上烷烃低温分子氧氧化  

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

作　　者：田鹏[1] 许磊[1] 黄韬[1] 谢鹏[1] 刘中民[1] 

机构地区：[1]中国科学院大连化学物理研究所,大连116023

出　　处：《高等学校化学学报》2002年第4期656-660,共5页Chemical Journal of Chinese Universities

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．MeAlPO-5, MeAPSO-35, MeAlPO-l8 and MeAPSO-18(Me=Co, Mn) were prepared by hy-drothermal synthesis and were characterized by XRD and 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 MeAPSO was higher thanthat over the same type MeAlPO molecular 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.

关 键 词：杂原子分子筛 氧气 烷烃 氧化 钴 锰 反应机理 催化剂 

分 类 号：O623.11[理学—有机化学] O643.36[理学—化学]