4.3 Article

New Ru PNP complexes as in situ Ru-oxo precursors in styrene and octane oxidation

期刊

JOURNAL OF COORDINATION CHEMISTRY
卷 75, 期 9-10, 页码 1129-1146

出版社

TAYLOR & FRANCIS LTD
DOI: 10.1080/00958972.2022.2110867

关键词

PNP ligands; Ru-oxo Species; CH bond activation; CC bond cleavage; alkane oxidation; styrene oxidation

资金

  1. NRF [111660]
  2. UKZN (URF)

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In this study, three ruthenium complexes were synthesized and characterized for the oxidation reactions of n-octane and styrene with different hybridizations of CH bonds. Ru-oxo species were found to act as active catalysts in the reactions, but exhibited different catalytic behaviors in the chosen models. These complexes are promising candidates for catalyzing C-1 partial oxidation and producing octanal and 1-octanol with high selectivity, which are in high demand in the industry.
The ruthenium complexes, [Ph2PN(R)PPh2](2)RuCl2, where R = C6H11 (a); C3H7 (b); C5H11 (c), have been synthesized and characterized. These complexes were studied for n-octane and styrene oxidation with different hybridizations of CH bonds. Ru-oxo species were identified as active species in both reactions but showed very different catalytic behavior in the chosen catalytic models. These complexes were good candidates to catalyze C-1 partial oxidation and result in high selectivity to octanal and 1-octanol, which have high industrial demand as precursors to alpha-octene (a good elasticizer for the polymer industry). Slight modification of the ligand backbone influenced both the rate of Ru-oxo formation and their nature. This resulted in different selectivity and conversion in both the studied oxidative reactions. These studies provide insights regarding the role and the mode of action of metal-oxo species during oxidation reactions, which is of interest to researchers in the field of homogenous catalysis.

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