Four alkoxohexavanadate-based pd-polyoxovanadates as robust heterogeneous catalysts for oxidation of benzyl-alkanes

Ji Kun Li; Xian Qiang Huang; Song Yang; Hong Wei Ma; Ying Nan Chi; Chang Wen Hu

doi:10.1021/ic502447b

Four alkoxohexavanadate-based pd-polyoxovanadates as robust heterogeneous catalysts for oxidation of benzyl-alkanes

Ji Kun Li, Xian Qiang Huang, Song Yang, Hong Wei Ma, Ying Nan Chi^*, Chang Wen Hu

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

78 Citations (Scopus)

Abstract

Four alkoxohexavanadate-based Pd-POVs [Pd(dpa)(acac)]₂[V₆O₁₃(OMe)₆] (1), [Pd(dpa)(acac)]₂[V₆O₁₁(OMe)₈] (2), [Pd(dpa)(acac)]₂[V₆O₁₁(OMe)₈]·H₂O (3), and [Pd(DMAP)₂(acac)]₂[V₆O₁₁(OMe)₈]·H₂O (4) (POV = polyoxovanadate; dpa = 2,2′-dipyridine amine; DMAP = 4-dimethylaminopyridine; acac = acetylacetone anion) have been synthesized and fully characterized by single crystal X-ray diffraction and powder X-ray diffraction analyses, Fourier transform infrared spectroscopy, element analyses, and X-ray photoelectron spectroscopy. In 1-4, Pd complexes and hexavanadate anions are assembled through electrostatic interactions. Interestingly, the [V₆O₁₁(OMe)₈]^2- cores in 2 and 3 are a pair of isomers that can be isolated by controlling crystallization temperature. Moreover, to the best of our knowledge, the {V6} core in 3 represents a new octamethoxyhexavanadates cluster. It is notable that compounds 1-4 exhibit excellent heterogeneous catalytic performance in the oxidation of benzyl-alkanes with t-butylhydroperoxide as oxidant. Among them, the catalytic activity of 1 (conv. and selec. up to 99%, respectively) outperforms others and can be reused without losing its activity.

Original language	English
Pages (from-to)	1454-1461
Number of pages	8
Journal	Inorganic Chemistry
Volume	54
Issue number	4
DOIs	https://doi.org/10.1021/ic502447b
Publication status	Published - 16 Feb 2015

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title = "Four alkoxohexavanadate-based pd-polyoxovanadates as robust heterogeneous catalysts for oxidation of benzyl-alkanes",

abstract = "Four alkoxohexavanadate-based Pd-POVs [Pd(dpa)(acac)]2[V6O13(OMe)6] (1), [Pd(dpa)(acac)]2[V6O11(OMe)8] (2), [Pd(dpa)(acac)]2[V6O11(OMe)8]·H2O (3), and [Pd(DMAP)2(acac)]2[V6O11(OMe)8]·H2O (4) (POV = polyoxovanadate; dpa = 2,2′-dipyridine amine; DMAP = 4-dimethylaminopyridine; acac = acetylacetone anion) have been synthesized and fully characterized by single crystal X-ray diffraction and powder X-ray diffraction analyses, Fourier transform infrared spectroscopy, element analyses, and X-ray photoelectron spectroscopy. In 1-4, Pd complexes and hexavanadate anions are assembled through electrostatic interactions. Interestingly, the [V6O11(OMe)8]2- cores in 2 and 3 are a pair of isomers that can be isolated by controlling crystallization temperature. Moreover, to the best of our knowledge, the {V6} core in 3 represents a new octamethoxyhexavanadates cluster. It is notable that compounds 1-4 exhibit excellent heterogeneous catalytic performance in the oxidation of benzyl-alkanes with t-butylhydroperoxide as oxidant. Among them, the catalytic activity of 1 (conv. and selec. up to 99%, respectively) outperforms others and can be reused without losing its activity.",

author = "Li, {Ji Kun} and Huang, {Xian Qiang} and Song Yang and Ma, {Hong Wei} and Chi, {Ying Nan} and Hu, {Chang Wen}",

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AU - Li, Ji Kun

AU - Huang, Xian Qiang

AU - Yang, Song

AU - Ma, Hong Wei

AU - Chi, Ying Nan

AU - Hu, Chang Wen

PY - 2015/2/16

Y1 - 2015/2/16

N2 - Four alkoxohexavanadate-based Pd-POVs [Pd(dpa)(acac)]2[V6O13(OMe)6] (1), [Pd(dpa)(acac)]2[V6O11(OMe)8] (2), [Pd(dpa)(acac)]2[V6O11(OMe)8]·H2O (3), and [Pd(DMAP)2(acac)]2[V6O11(OMe)8]·H2O (4) (POV = polyoxovanadate; dpa = 2,2′-dipyridine amine; DMAP = 4-dimethylaminopyridine; acac = acetylacetone anion) have been synthesized and fully characterized by single crystal X-ray diffraction and powder X-ray diffraction analyses, Fourier transform infrared spectroscopy, element analyses, and X-ray photoelectron spectroscopy. In 1-4, Pd complexes and hexavanadate anions are assembled through electrostatic interactions. Interestingly, the [V6O11(OMe)8]2- cores in 2 and 3 are a pair of isomers that can be isolated by controlling crystallization temperature. Moreover, to the best of our knowledge, the {V6} core in 3 represents a new octamethoxyhexavanadates cluster. It is notable that compounds 1-4 exhibit excellent heterogeneous catalytic performance in the oxidation of benzyl-alkanes with t-butylhydroperoxide as oxidant. Among them, the catalytic activity of 1 (conv. and selec. up to 99%, respectively) outperforms others and can be reused without losing its activity.

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Four alkoxohexavanadate-based pd-polyoxovanadates as robust heterogeneous catalysts for oxidation of benzyl-alkanes

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