Highly efficient divanadium(V) pre-catalyst for mild oxidation of liquid and gaseous alkanes

•New binuclear V(V) complex bearing an NO2-donor Schiff base ligand is synthesized.•This compound is highly active catalyst precursor in the oxidation of alkanes by H2O2.•2-Pyrazinecarboxylic acid acts as an efficient co-catalyst.•High yields (up to 45% based on alkanes) and TONs (up to 7800) are ac...

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Veröffentlicht in:Applied catalysis. A, General General, 2013-06, Vol.460-461, p.82-89
Hauptverfasser: Gupta, Samik, Kirillova, Marina V., Guedes da Silva, M. Fátima, Pombeiro, Armando J.L.
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Sprache:eng
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Zusammenfassung:•New binuclear V(V) complex bearing an NO2-donor Schiff base ligand is synthesized.•This compound is highly active catalyst precursor in the oxidation of alkanes by H2O2.•2-Pyrazinecarboxylic acid acts as an efficient co-catalyst.•High yields (up to 45% based on alkanes) and TONs (up to 7800) are achieved.•Oxidation proceeds via radical mechanism with participation of hydroxyl radicals. A new binuclear oxovanadium(V) complex bearing an NO2-donor Schiff base ligand, [{VO(EtO)(EtOH)}2(1κ2O,κN:2κ2O,κN-L)]·2H2O (H4L=bis(2-hydroxybenzylidene)oxalohydrazonic acid) was prepared and fully characterized by IR, 1H NMR and electronic spectroscopies, elemental analysis and single crystal X-ray diffraction. In the presence of 2-pyrazinecarboxylic acid (PCA) or another acid promoter, this compound acts as a highly efficient pre-catalyst towards the oxidation of gaseous and liquid alkanes by aqueous H2O2 under mild conditions, in aqueous MeCN. Total yields of oxygenates up to 45% and overall turnover numbers up to 7.8×103 are achieved.
ISSN:0926-860X
1873-3875
DOI:10.1016/j.apcata.2013.03.034