Abstract
The synthesis of RuCl(CO)(NO)L2 (L = PtBu2Me) and replacement of Cl- by BF4-, CO, CH3CN, H2O, F-, and H- are reported. NaBArF4 (ArF = 3,5-(CF3)2C6H3) removes halide to produce the four-coordinate 16-electron cation Ru(NO)(CO)L2+, shown by X-ray diffraction to have a nonplanar structure symptomatic of greater back bonding than isoelectronic Ru(CO)2L2. Variable-temperature 1H NMR studies of the tBu groups in [Ru(NO)(CO)L2](BArF4) show a ΔG⧧ (100 °C) for inversion through planar Ru of 19.1 kcal/mol. Ru(η1-BF4)(CO)(NO)L2 is shown by X-ray diffraction to have a square-pyramidal structure with apical bent NO. The IR frequencies of NO and CO are analyzed to conclude that all five-coordinate species except Ru(NO)(CO)2L2+ and RuH(NO)(CO)L2 have bent nitrosyls; these last two have linear NO. RuX(CO)(NO)(PH3)2+ (X = Cl-, BF4-, H-, no ligand, NCH, CO) was calculated with ab initio calculations at the Becke3LYP level. Depending on the nature of X, one minimum (square pyramid with bent NO) or two minima (square pyramid...
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