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Cationic D4R zinc phosphate-anionic polyoxometalate hybrids: synthesis, spectra, structure and catalytic studies

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Title Cationic D4R zinc phosphate-anionic polyoxometalate hybrids: synthesis, spectra, structure and catalytic studies
 
Creator KALITA, AC
ROCH-MARCHAL, C
MURUGAVEL, R
 
Subject HIGHLY EFFICIENT UTILIZATION
TRANSITION-METAL-COMPLEXES
HYDROGEN-PEROXIDE
SUBSTITUTED POLYOXOMETALATE
SELECTIVE EPOXIDATION
COORDINATION POLYMER
OXIDATION-RESISTANT
AUXILIARY LIGANDS
ALKENE OXIDATION
MOLECULAR-OXYGEN
 
Description A facile synthetic strategy for the generation of a new class of inorganic-organic-inorganic hybrids is reported. Replacement of labile DMSO ligands from the preformed Double-Four-Ring (D4R) zinc phosphate cluster [Zn(dipp){(CH3)(2)SO}](4) by the addition of 4-aminopyridine (4-ampyr) results in the isolation of another discrete D4R cluster [Zn(dipp)(4-ampyr)](4) (1), which forms a hydrogen-bonded framework in solid-state. If 1-methyl-4,4'-bipyridinium salts are employed instead, tetra-cationic D4R cluster [Zn(dipp)-(L)](4)[PF6](4) (2) and [Zn(dipp)(L)](4)[ClO4](4) (3) (L = 1-methyl-4,4'-bipyridinium, dipp = 2,6-di-iso-propylphenyl-phosphate) are isolated. Compound 2 was reacted with three different polyoxometalates, [TBA](4)[Mo8O26] (POM-1), [TBA](4)[PMo11VO40] (POM-2), and [TBA](4)[SiMo12O40] (POM-3) to obtain amorphous hybrids, [Zn(dipp)(L)](4)[Mo8O26] (4), [Zn(dipp)(L)](4)[PMo11VO40] (5), and [Zn(dipp)(L)](4)[SiMo12O40] (6), respectively. All the hybrid materials have been characterized by analytical and spectroscopic studies. The molecular structure of 1 has also been determined by single-crystal XRD measurements. N-2 gas sorption analyses show moderate BET surface area and also establish the mesoporous nature of the hybrids 4-6. The catalytic potential of hybrids 4, 5 and 6 has been explored towards epoxidation of cyclohexene.
 
Publisher ROYAL SOC CHEMISTRY
 
Date 2014-10-16T07:07:42Z
2014-10-16T07:07:42Z
2013
 
Type Article
 
Identifier DALTON TRANSACTIONS, 42(26)9755-9763
http://dx.doi.org/10.1039/c3dt50786f
http://dspace.library.iitb.ac.in/jspui/handle/100/15512
 
Language en