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Abstract

Infrared multiple photon dissociation spectroscopy (IR‐MPD) has been employed to determine the nature of CO₂ binding to size‐selected platinum cluster anions, Pt_n^- (n=4–7). Interpreted in conjunction with density functional theory simulations, the results illustrate that the degree of CO₂ activation can be controlled by the size of the metal cluster, with dissociative activation observed on all clusters n≥5. Of potential practical significance, in terms of the use of CO₂ as a useful C1 feedstock, CO₂ is observed molecularly‐bound, but highly activated, on the Pt₄^- cluster. It is trapped behind a barrier on the reactive potential energy surface which prevents dissociation.