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- W3006340452 endingPage "4334" @default.
- W3006340452 startingPage "4324" @default.
- W3006340452 abstract "Evaluation of the hemilability of hybrid ligands provides a key to understand the metal-ligand cooperation in transition metal catalysis. Here, we design and synthesize a type of RuII complexes based on the hemilability of N-heterocyclic carbenes (NHCs), pyridine, and pyrazole, to compare their activity with other reported Ru catalysts in benzylic C-H oxidation. The RuII catalysts showed ultrastrong catalytic activity in water at room temperature and achieved a turnover frequency (TOF) of 114 h-1, which is the highest TOF value ever reported for Ru-catalyzed benzylic C-H oxidation. The addition of tridentate hybrid ligands in the Ru central position has two beneficial effects: NHCs with a stronger donor ability stabilize the Ru center; however, nitrogen ligands with a relatively weaker donor ability release from the Ru center, so that they induce a reaction. UV-vis, high-resolution electrospray ionization mass spectrometry (ESI-MS), electron paramagnetic resonance (EPR) spectrometry, the trapping of radicals, and the density functional theory calculations (DFT) suggested that a cation catalyst L-RuII-tBuO2H is formed via the reaction between starting RuII catalysts and tert-butyl hydroperoxide, which further undergoes a cleavage of the O-O bond to generate a radical and a cation L-RuIII-OH active intermediate." @default.
- W3006340452 created "2020-02-24" @default.
- W3006340452 creator A5013789507 @default.
- W3006340452 creator A5033684035 @default.
- W3006340452 creator A5044331701 @default.
- W3006340452 creator A5061314860 @default.
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- W3006340452 creator A5071296084 @default.
- W3006340452 creator A5076454806 @default.
- W3006340452 creator A5084055182 @default.
- W3006340452 date "2020-02-11" @default.
- W3006340452 modified "2023-10-02" @default.
- W3006340452 title "Highly Active and Robust Ruthenium Complexes Based on Hemilability of Hybrid Ligands for C–H Oxidation" @default.
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