We have used the large electric fields at the interface of a Pt(111) electrode and an acetonitrile electrolyte solution to tune the interaction between adsorbed CO and the Pt(111) surface. The electrode potential is varied over a 2.5 Volt range. As the electrode potential is made more positive, the CO vibrational frequency increases and the vibrational lifetime decreases. Over the potential range investigated, the tuning is about 35-40 cm(-1) and the lifetime varies from approximate to 2.1 to approximate to 1.5 ps. Ab initio calculations performed for CO/Cu(100) predicted the opposite trend for the lifetimes for that system [M. Head-Gordon and J. C. Jully, Chem. Phys. 175, 37 (1993)]. Within an empirical model of nonadiabatic charge transfer [B. N. J. Persson and M. Persson, Solid State Commun. 36, 175 (1980)], our observations can be explained by a decreasing 2 pi-derived density of states of the Pt/CO complex at the Fermi level.