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The application of cationic Ru(II)‐CNC pincer complexes [Ru(CNC)(CO)(PPh3)Cl]PF6 (1), [Ru(CNC)(PPh3)2Cl]PF6 (2), [Ru(CNC)(η2:η2‐COD)Cl]PF6 (4), and [Ru(CNC)(DMSO)2Cl]PF6 (5) in acceptorless dehydrogenation of alcohols is reported under conventional “oil‐bath” and microwave heating conditions. The effect of different ancillary ligands (CO, PPh3, COD, and DMSO) have been demonstrated during catalysis. Complexes with more π‐acid ligands CO and COD perform better compared with those with PPh3 and DMSO ligands. A plausible mechanism is proposed based on NMR and mass investigation during the catalysis. The catalytic performance matches with the order of trans effect among the four ancillary ligands studied in these complexes. Further, a significant reduction in reaction time, as well as reaction temperature, was observed for catalytic reactions under the microwave‐assisted reaction compared with the oil‐bath heating reaction.

A series of Ru(III)-NHC complexes, identified as [RuIII(PyNHCR)(Cl)3(H2O)] (1a-c), have been prepared, starting from RuCl3·3H2O following a base-free route. The Lewis acidic Ru(III) centre operates via a halide-assisted, electrophilic C-H...

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