CO2 Activation and Hydrogenation by PtHn- Cluster Anions

摘要

Gas phase reactions between PtHn- cluster anions and CO2 were investigated by mass spectrometry, anion photoelectron spectroscopy, and computations. Two major products, PtCO2H- and PtCO2H3-, were observed. The atomic connectivity in PtCO2H- can be depicted as HPtCO2, where the platinum atom is bonded to a bent CO2 moiety on one side and a hydrogen atom on the other. The atomic connectivity of PtCO2H3- can be described as H2Pt(HCO2)(-), where the platinum atom is bound to a formate moiety on one side and two hydrogen atoms on the other. Computational studies of the reaction pathway revealed that the hydrogenation of CO2 by PtH3- is highly energetically favorable.