C-H Bond Activation by a Ruthenium(II) β- diketonate Complex: A Mechanistic Study (CROSBI ID 253550)
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Podaci o odgovornosti
Briš, Anamarija ; Turel, Iztok ; Roithová, Jana
engleski
C-H Bond Activation by a Ruthenium(II) β- diketonate Complex: A Mechanistic Study
Ruthenium(II)-catalysed C-H bond activation of arenes containing a functional directing group depends on the ligand coordinated to ruthenium(II). In this study, 2-phenylpyridine C-H activation catalysed by a “piano-stool” ruthenium(II) complex containing a fluorinated β-diketonate ligand was examined by ESI-MS in combination with CID experiments. [Ru(β- diketonate)(CTPhPy)Cl]^+ was identified as an active intermediate, and its collisional activation leads to C-H activation. CID analysis indicates proton transfer from the phenylpyridine to the chlorine anion, showing HCl elimination, while the β-diketonate ligand is retained in the complex together with the activated phenylpyridine. Furthermore, DFT calculations were performed for the neutral analogue [Ru(β-diketonate)(PhPy)Cl] to identify all ruthenium intermediates along the C-H activation reaction pathway. The results suggest that the most stable structure of [Ru(β-diketonate)(PhPy)Cl] has pre-activated 2- phenylpyridine with a partly developed Ru-H bond. Further, we show that K_2CO_3 is not directly involved in the C-H activation step and it serves in the reaction as a base.
Ruthenium ; Mass spectrometry ; C-H activation ; Collision-induced dissociation ; Charge-tagging method
Charles University Research Centre program No. UNCE/SCI/014
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Podaci o izdanju
2018 (44)
2018.
6107-6113
objavljeno
1434-193X
1099-0690
10.1002/ejoc.201800787
Povezanost rada
Kemija