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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(英文)

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

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【作者】 袁霞罗和安李芳

【Author】 YUAN Xia, LUO He-an1, LI Fang (College of Chemical Engineering, Xiantan University, Xiangtan, 411105, China)

【机构】 湘潭大学化工学院湘潭大学化工学院 湖南湘潭411105湖南湘潭411105

【摘要】 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0.85MPa的氧压下,150℃反应3h,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.

【Abstract】 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.

【关键词】 Cosalen分子筛封装氧气环己烷氧化
【Key words】 CosalenZeoliteEncapsulationOxygenCyclohexane oxidation
【基金】 Project(04JJ3042)supported by the Hunan Provincial Natural Science Foundation of China.
  • 【文献出处】 分子催化 ,Journal of Molecular Catalysis , 编辑部邮箱 ,2007年01期
  • 【分类号】O641.4
  • 【被引频次】14
  • 【下载频次】353
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