Three Pd-decavanadates with a controllable molar ratio of Pd to decavanadate and their heterogeneous aerobic oxidation of benzylic C–H bonds.

Three Pd-decavanadates with a controllable molar ratio of Pd to decavanadate and their heterogeneous aerobic oxidation of benzylic C–H bonds.
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三种钯与十钒酸盐摩尔比可控的十钒酸盐及其对苄基 C–H 键的非均相好氧氧化

DOI:
10.1039/c7dt03898d
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发表时间:
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期刊:
Dalton Trans.
影响因子:
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通讯作者:
Changwen Hu
Changwen Hu
中科院分区:
其他
文献类型:
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作者:
Xianqiang Huang;Jikun Li;Guodong Shen;Nana Xin;Zhengguo Lin;Yingnan Chi;Jianmin Dou;Dacheng Lia;Changwen Hu

文献摘要

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通过钯配合物与[V10 O28]6-的结合,合成了三种钯十钒酸盐化合物[Pd(NH3)4]3[V10 O28]·8H 2 O(1),[Pd(deta)(H2O)]2(NH 4)2[V10 O28]·2 H2O(2),(deta =二亚乙基三胺)和[Pd(dpa)2](Hdpa)2(Et 3 NH)2[V10 O28]·2 H2O(3)(dpa = 2,2 ′-二吡啶胺)的合成,并通过单晶X射线衍射(SXRD)、粉末X射线衍射(PXRD)、红外光谱(FT-IR)和元素分析(EA)对其进行了表征。有趣的是,在这三种化合物中,通过改变N-配体,Pd与十钒酸盐的摩尔比从3:1变化到1:1。    三种钯十钒酸盐作为非均相催化剂,在无溶剂条件下,不添加任何助剂和助催化剂,对苄型烃的有氧氧化反应具有活性。此外,化合物1可以重复使用三次而不会失去其活性。
By the combination of Pd-complexes and [V10O28]6−, three Pd-decavanadate compounds [Pd(NH3)4]3[V10O28]·8H2O (1), [Pd(deta)(H2O)]2(NH4)2[V10O28]·2H2O (2) (deta = diethylenetriamine) and [Pd(dpa)2](Hdpa)2(Et3NH)2[V10O28]·2H2O (3) (dpa = 2,2′-dipyridylamine) have been successfully synthesized and thoroughly characterized using single X-ray diffraction (SXRD), powder X-ray diffraction (PXRD), infrared spectroscopy (FT-IR) and elemental analyses (EA). Interestingly, in the three compounds, the molar ratios of Pd to decavanadate vary from 3 : 1 to 1 : 1 by changing N-ligands. The three Pd-decavanadates as heterogeneous catalysts are active in the aerobic oxidation of benzylic hydrocarbons under solvent-free conditions without adding any additives and co-catalysts. Moreover, compound 1 can be reused three times without losing its activity.