NaBAr4F (sodium tetrakis[(3,5-trifluoromethyl)phenyl]borate) was found to catalyze reactions of (Phebox)Ir-III-(acetate) (Phebox = 2,6-bis(4,4-dimethyloxazolinyl)-3,5-dimethylphenyl) complexes, including (i) beta-H elimination of (Phebox)Ir(OAc)(n-alkyl) to give (Phebox)Ir(OAc)(H) and the microscopic reverse, alkene insertion into the Ir H bond of (Phebox)Ir(OAc)(H), and (ii) hydrogenolysis of the Ir-alkyl bond of (Phebox)Ir(OAc)(n-alkyl) and the microscopic reverse, C H activation by (Phebox)Ir(OAc) (H), as indicated by H/D exchange experiments. For example, beta-H elimination of (Phebox)Ir(OAc)(n-octyl) (2-Oc) proceeded on a time scale of minutes at -15 degrees C in the presence of (0.4 mM) NaBAr4F as compared with a very slow reaction at 125 degrees C in the absence of NaBArF4. In addition to NaBAr4F, other Lewis acids are also effective. Density functional theory calculations capture the effect of the Nal" cation and indicate that it operates primarily by promoting kappa(2) - kappa(1) dechelation of the acetate anion, which opens the coordination site needed to allow the observed reaction to proceed. In accord with the effect on these individual stoichiometric reactions, NaBAr4F was also found to cocatalyze, with (Phebox)Ir(OAc)(H), the acceptorless dehydrogenation of n-dodecane.