First-Principles study of Hydrogen, Carbon, Nitrogen, and Oxygen atoms adsorption on PuO₂(110) surfaces

Abstract The investigation into the adsorption behavior of atoms of hydrogen, carbon, nitrogen, and oxygen located on the (110) face of plutonium dioxide (PuO 2 ) utilizing the projector augmented wave (PAW) method, coupled with density functional theory (DFT) incorporating on-site Coulombic interaction corrections (GGA+U), reveals a spectrum of adsorption tendencies. Within this framework, a nuanced interplay emerges, showcasing both weak and robust binding affinities with the PuO 2 (110) surface. Detailed scrutiny of the charge density differences (CDD) and partial density of states (PDOS) at strategic adsorption locales unveils distinct mechanisms governing these interactions. Specifically, electrostatic forces emerge as the driving factor behind the weaker associations, while the more substantial adhesions are characterized by the presence of covalent bonding. This comprehensive analysis not only delineates the diversity in adsorption behaviors but also underscores the multifaceted nature of surface interactions on PuO 2 (110), providing valuable insights into the underlying physics governing such phenomena.