Ammoximation of cyclohexanone in acetic acid using titanium silicalite-1 catalyst: Activity and reaction pathway
Ammoximation of cyclohexanone in acetic acid using titanium silicalite-1 catalyst: Activity and reaction pathway
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DOI：
10.1016/j.molcata.2005.04.014
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发表时间：
2005-07
影响因子：
--
通讯作者：
T. Sooknoi;Veerachai Chitranuwatkul
中科院分区：
文献类型：
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作者：
T. Sooknoi;Veerachai Chitranuwatkul
以乙酸为溶剂，在60℃下研究了钛硅分子筛（TS-1）的活性以及环己酮氨肟化生产环己酮肟的反应路径。还评估了溶剂、氮源、水含量和活性位点稳定性的影响。研究发现，在以乙酸为溶剂的反应中，环己酮的氨肟化主要通过亚胺的氧化进行，而亚胺主要是由酮与氨缩合原位形成的。此外，弱酸的铵盐，例如乙酸盐、柠檬酸盐和碳酸盐，可以用作乙酸氨肟化的氮源。水被证明可以抑制亚胺的形成，并防止副反应。此外，TS-1具有优异的稳定性，可以重复使用而不会明显损失活性。
The activity of titanium silicalite (TS-1) and the reaction pathway for the ammoximation of cyclohexanone to produce cyclohexanone oxime were studied using acetic acid as a solvent at 60°C. The effect of solvent, sources of nitrogen, water content and the active site stability were also evaluated. It was found that, in the reaction using acetic acid as a solvent, the ammoximation of cyclohexanone proceeded mainly via the oxidation of imine, which was primarily formed in situ by the condensation of ketone with ammonia. In addition, the ammonium salts of weak acids, such as acetate, citrate and carbonate, can be used as nitrogen sources for the ammoximation in acetic acid. Water was shown to inhibit the formation of imine, and also prevent the side reactions. Moreover, TS-1 possessed an excellent stability, and can be reused without significant loss of activity.