分子筛负载席夫碱钴配合物的制备及其催化氧气氧化环己烷

采用柔性配位法将双水杨醛叉乙二胺合钴(Cosalen)封装到了NaY分子筛的超笼中,采用FT-IR,UV-Vis,XRD,TG/DTA 和 BET比表面积及孔容分析对负载型配合物(Cosalen-NaY)进行了表征.在催化氧气氧化环己烷的反应过程中,Cosalen-NaY能有效地促进环己基过氧化物的分解,在0.85 MPa的氧压下,150 ℃反应3 h,环己烷的转化率达到13.4%,在反应体系中加入乙腈作溶剂,130 ℃下进行反应,环己烷的转化率提高到{28.3%.产物中环己醇、环己酮、己二酸的选择性明显高于Cosalen为催化剂的反应.催化剂回收实验表明Cosalen-NaY经过三次重复使用后,没有显著的活性组分流失,可以重复使用.

Preparation of Zeolite Encapsulated Cobalt Schiff Base and Catalytic Activity in Cyclohexane Oxidation by Oxygen

N,N'-bis (salicylidene) ethylenediiminocobalt (Cosalen) has been successfully encapsulated into Microporous NaY zeolite by the flexible ligand method, which were characterized by FT-IR, UV-Vis, XRD, TG/DTA and BET Surface areas analysis. As catalyst for the oxidation of cyclohexane using oxygen, Cosalen-NaY showed the strong ability to decompose cyclohexyl hydroperoxide (CHHP) and the better selectivity for cyclohexanol, cyclohexanone and adipic acid than the neat complex. The conversion of cyclohexane reached 13.4% at 423 K under oxygen pressure 0.85 MPa for 3 h. After adding CH3CN as solvent, the conversion was up to 28.3% even at 403 K. Recycling test showed that the catalyst can be used repeatedly with the neglected loss of active site.