Catalytic oxidation of cyclohexane to cyclohexanone and cyclohexanol by oxygen in a solvent-free system over metal-containing ZSM-5 catalysts
Catalytic oxidation of cyclohexane to cyclohexanone and cyclohexanol by oxygen in a solvent-free system over metal-containing ZSM-5 catalysts
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DOI：
10.1016/j.apcata.2006.02.037
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发表时间：
2006-05
影响因子：
5.5
通讯作者：
H.-X. Yuan;Q. Xia;H. Zhan;Xinhuan Lu;K. Su
中科院分区：
文献类型：
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作者：
H.-X. Yuan;Q. Xia;H. Zhan;Xinhuan Lu;K. Su
在无溶剂体系中，用分子氧在含金属的ZSM-5催化剂上多相氧化环己烷。在所测试的M-ZSM-5和M/ZSM-5催化剂中，含Co的ZSM-5催化剂包括Co/ZSM-5（通过离子交换和煅烧制备）和Co-ZSM-5（通过离子交换和干燥制备）显示出最好的环己烷氧化为环己酮和环己醇的活性。Co/ZSM-5催化剂对环己烷的氧化活性与Co-ZSM-5催化剂基本相同，但Co-ZSM-5催化剂中的钴容易浸出。Co/ZSM-5（焙烧）催化剂在393 K、1.0MPa氧气压力下，环己烷转化率可达10mol%左右，KA油（环己酮和环己醇的混合物）选择性可达97%。考察了反应温度、反应压力、反应时间、金属种类、叔丁基过氧化氢（TBHP）的加入量以及催化剂的重复使用等因素对反应的影响。对于标题氧化，Co/ZSM-5是可回收的，并且可以表现为真正的非均相催化剂。
Heterogeneous oxidation of liquid cyclohexane by molecular oxygen was carried out over metal-containing ZSM-5 catalysts in a solvent-free system. Among those M-ZSM-5 and M/ZSM-5 catalysts tested, Co-containing ZSM-5 catalysts including Co/ZSM-5 (prepared by ion-exchange and calcination) and Co-ZSM-5 (prepared by ion-exchange and drying) showed the best activity for the oxidation of cyclohexane to cyclohexanone and cyclohexanol. Co/ZSM-5 had almost the same activity as Co-ZSM-5 for the cyclohexane oxidation; however, the leaching of cobalt from Co-ZSM-5 readily occurred. Co/ZSM-5 (calcined) catalyst could achieve about 10mol% conversion of cyclohexane and 97% selectivity of KA-oil (the mixture of cyclohexanone and cyclohexanol) at 393K under the pressure of 1.0MPa O2. In addition, other factors like the temperature, the pressure, the time, various metals, the tert-butylhydroperoxide (TBHP) addition, and the catalyst reuse were investigated carefully. For the titled oxidation, Co/ZSM-5 was recyclable, and could behave as a truly heterogeneous catalyst.