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Copper-Containing Polyoxometalate-Based Metal-Organic Frameworks as Highly Efficient Heterogeneous Catalysts toward Selective Oxidation of Alkylbenzenes.
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2019-11-13 , DOI: 10.1021/acs.inorgchem.9b02189
Dandan Li 1 , Xinyi Ma 1 , Quanzhong Wang 1 , Pengtao Ma 1 , Jingyang Niu 1 , Jingping Wang 1
Affiliation  

With a one-pot assembly method, two copper-containing Keggin-type polyoxometalate-based metal-organic frameworks (POMOFs), i.e., [CuI6(trz)6{PW12O40}2] (HENU-2, HENU = Henan University; trz = 1,2,4- triazole) and [CuI3(trz)3{PMo12O40}] (HENU-3), were successfully prepared and structurally characterized. These two compounds, which are generated by the extension of a crown-like {Cu6(trz)6} macrocycle-based sandwich-type structural unit, possess identical noninterpenetration 3D frameworks except for the polyanions difference. Additionally, both of themare assessed as highly effective heterogeneous catalysts in facilitating the oxidation of alkylbenzenes to ketone products in the presence of tert-butyl hydroperoxide. Under optimized conditions, HENU-2 can achieve a 95.2% conversion of diphenylmethane in 20 h with a 100% selectivity toward benzophenone, and it was reused for three runs with constant high activity, which outperforms most POM-based catalysts for this catalytic reaction.

中文翻译:

含铜的多金属氧酸盐基金属有机骨架作为烷基苯选择性氧化的高效多相催化剂。

使用一锅法组装时,两个含铜的Keggin型多金属氧酸盐基金属有机框架(POMOF),即[CuI6(trz)6 {PW12O40} 2](HENU-2,HENU =河南大学; trz = 1,2,4-三唑)和[CuI3(trz)3 {PMo12O40}](HENU-3)已成功制备并进行了结构表征。通过扩展基于冠状的{Cu6(trz)6}大环基夹心型结构单元而生成的这两种化合物具有相同的非互穿3D框架,除了聚阴离子的差异。另外,在叔丁基氢过氧化物存在下,它们都被认为是促进烷基苯氧化为酮产物的高效多相催化剂。在最佳条件下,HENU-2在20小时内可实现95.2%的二苯甲烷转化率,且对二苯甲酮的选择性为100%,
更新日期:2019-11-14
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