Citation: SUN Bo, LIU Hai-Feng, SONG Hai-Feng, ZHENG Hui. Microdynamics Simulations of the Hydrogen-Corrosion Resistance of Passivation Layers on Pu Surface[J]. Acta Physico-Chimica Sinica, ;2015, 31(S1): 81-89. doi: 10.3866/PKU.WHXB2014Ac16 shu

Microdynamics Simulations of the Hydrogen-Corrosion Resistance of Passivation Layers on Pu Surface

1.
Institute of Applied Physics and Computational Mathematics, Beijing 100094, P. R. China

Corresponding author: SUN Bo,
Fund Project: 中国工程物理研究院科学技术发展专项基金(9090707)资助项目 (9090707)

Based on the non-local van der Waals density functional (vdW-DF)+U scheme, we have performed a first-principles molecular dynamics (FPMD) study of the interaction dynamics for H₂ impingement against the Pu oxide (PuO₂) and Pu nitride (PuN) passivation layers on Pu metal surface. Results show that, except for weak physisorption, both the PuO₂ and PuN surfaces are so difficult to access that almost all of the H₂ molecules will bounce back to the vacuum when their initial kinetic energies are not sufficient. Although dissociative adsorption of H₂ on PuO₂ surfaces is found to be very exothermic, the collision-induced dissociation barriers of H₂ are calculated to be very high. Unfortunately, PuO₂ can be reduced to α-Pu₂O₃ under oxygen-lean conditions. Molecular H₂ can easily penetrate and diffuse in α-Pu₂O₃, and, as a result, α-Pu₂O₃ can promote the hydrogenation of Pu metal. Unlike PuO₂, PuN is found to be a stable and uniform passivation layer against hydrogen-corrosion of Pu, and the interacting system of PuN and H is shown to be thermodynamically unstable. Overall, the current study reveals the different hydrogen-corrosion resistances of PuO₂ and PuN passivation layers, which have implications for the interpretation of experimental observations and will be helpful to understand the surface corrosion and passivation of Pu metal.
- Surface passivation,
- Plutonium oxide,
- Plutonium nitride,
- Surface hydrogen-corrosion,
- First-principles molecular dynamics
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