钚表面钝化层抗氢蚀机理的微观动力学模拟

doi:10.3866/PKU.WHXB2014Ac16

Abstract

Abstract:

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.

Key words: Surface passivation, Plutonium oxide, Plutonium nitride, Surface hydrogen-corrosion, First-principles molecular dynamics

MSC2000:

O647

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 Phys. -Chim. Sin., 2015, 31(Suppl): 81-89.

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

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