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Radiolytic corrosion of actinide materials represent an issue for the long term storage and disposal of nuclear materials. Molecular species adsorbed at the surface of the actinides may impact the rate of radiolysis, and as the surfaces corrode, the soluble toxic and radioactive species leach into groundwater. It is therefore critical to characterise the surface composition of actinides. Here, we employ ab initio modelling to determine the surface composition of PuO2 with respect to adsorbed CO2. We found that CO2 interacts strongly wit