Microwave-assisted one-pot functionalization of metal–organic framework MIL-53(Al)-NH2 with copper(II) complexes and its application in olefin oxidation,Catalysis Science & Technology

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Microwave-assisted one-pot functionalization of metal–organic framework MIL-53(Al)-NH2 with copper(II) complexes and its application in olefin oxidation
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2017-11-13 00:00:00 , DOI: 10.1039/c7cy01941f
T. Bunchuay _{1,

2,

3,

4,

5} , R. Ketkaew _{6,

7,

8,

9,

10} , P. Chotmongkolsap _{1,

2,

3,

4,

5} , T. Chutimasakul _{1,

2,

3,

4,

5} , J. Kanarat _{1,

2,

3,

4,

5} , Y. Tantirungrotechai _{6,

7,

8,

9,

10} , J. Tantirungrotechai _{1,

2,

3,

4,

5}

Affiliation

A simple, rapid, and efficient functionalization of the metal–organic framework MIL-53(Al)-NH₂ with copper(II) complexes by microwave irradiation is described. The one-pot post-synthetic modification was based on the Schiff base reaction between the aldehyde added and the primary aryl amino group in the organic linker of MIL-53(Al)-NH₂, which afforded coordination sites for copper(II). The effects of synthetic parameters such as solvent, reaction time, and reactant ratio were evaluated. The functionalized materials were structurally characterized and examined for potential applications in catalysis. The copper complex functionalized MIL-53(Al) was active towards the oxidation of olefins with tert-butyl hydroperoxide as an oxidant. The results showed that if the olefin possessed allylic hydrogens such as cyclohexene, allylic oxidation products were obtained, but epoxide was the major product obtained from terminal olefins without allylic hydrogens. The reaction mechanism based on density functional theory calculations provides some insights into the observed experimental results.

中文翻译：

微波辅助金属一有机骨架MIL-53（Al）-NH ₂与铜（II）配合物的一锅功能化及其在烯烃氧化中的应用

描述了通过微波辐射对金属-有机骨架MIL-53（Al）-NH ₂与铜（II）配合物的简单，快速和有效的官能化。一锅合成后的修饰基于添加的醛与MIL-53（Al）-NH ₂的有机连接基中的伯芳基氨基之间的席夫碱反应，该席夫碱提供了铜（II）的配位点。评估了诸如溶剂，反应时间和反应物比例之类的合成参数的影响。对功能化的材料进行结构表征，并检查其在催化中的潜在应用。铜络合物官能MIL-53（Al）的活性是用对烯烃氧化叔丁基过氧化氢作为氧化剂。结果表明，如果烯烃具有烯丙基氢，例如环己烯，则获得烯丙基氧化产物，但是环氧化物是由没有烯丙基氢的末端烯烃获得的主要产物。基于密度泛函理论计算的反应机理为观察到的实验结果提供了一些见识。

更新日期：2017-11-22

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