Monday, June 30, 2008
Emerald Grand Ballroom (Sheraton Burlington Hotel and Conference Center)
224

Dynamics of the Reactions of Some Pentakis(alkylisocyanide)Cobalt(II) Complexes with Triarylphosphines

Olayinka A. Oyetunji, Godiraone Ramokongwa, and Clifford A. L. Becker. University of Botswana, Gaborone, Botswana

Many organoisocyanide cobalt(I,II, & III) complexes that have been reported in literature exist as five-coordinate complexes. While the thermodynamics and kinetics of complex formation and ligand substitution of octahedral transition metal complexes have been widely studied, similar studies on five-coordinate square pyramidal or trigonal bipyramidal transition metal complexes have received significantly less attention. This study looks at the reactions of some five-coordinate isocyanide cobalt(II) complexes with the aim of providing information on the relative rates and mechanisms of the reactions.

The progress of the reactions of [Co(CNC8H17-t)5](ClO4)2 (A) and [Co2(CNCHMe2)10](ClO4)4.5H2O {reacting as [Co(CNCHMe2)5]2+ (B) in solution} with PPh3 and P(C6H4Me-p)3 was monitored by both infrared and UV-Visible spectroscopic techniques. Both Co(II) complexes react with the tri-aryl phosphines leading to complex kinetics. In all reactions, a fast substitution of A and B by the phosphines is first observed and this is followed by slower reduction of the substituted Co(II) to Co(I). After the substitution, a 4:1(isocyanide:phosphine) Co(I) complex is apparently formed initially and then undergoes further substitution with excess phosphine to produce a final 3:2(isocyanide:phosphine) pentakis Co(I) complex. The isopropylisocyanide-cobalt(II) complex B reacts with P(C6H4Me-p)3 leading to immediate disproportionation of B to Co(III) and Co(I). The final product is however a 3:2 Co(I) complex.

Kinetic studies on the slower reduction of the complexes to Co(I) produce complex results as it is evident that the reactions involve disproportionation and re-arrangement among others. However the first fast substitution process was followed using the stopped-flow technique. Steric hindrance seems to play a significant role in these reactions as B reacts faster with the phosphines than A does. For example, at 25oC, B reacts with PPh3 with second order rate constant (k2) of (1.29±0.03) x 103 M-1 s-1 while A reacts with the same phosphine with k2 = (9.42±0.16) x 102 M-1 s-1.