In:
Chinese Physics B, IOP Publishing, Vol. 30, No. 2 ( 2021-02-01), p. 026601-
Abstract:
First principles calculation is performed to study the co-adsorption behaviors of O 2 and CO 2 on δ -Pu(100) surface by using a slab model within the framework of density functional theory (DFT). The results demonstrate that the most favorable co-adsorption configurations are T v -C 4 O 7 and T p1 -C 2 O 8 , with adsorption energy of –17.296 eV and –23.131 eV for CO 2 -based and O 2 -based system, respectively. The C and O atoms mainly interact with the Pu surface atoms. Furthermore, the chemical bonding between C/O and Pu atom is mainly of ionic state, and the reaction mechanism is that C 2s, C 2p, O 2s, and O 2p orbitals overlap and hybridize with Pu 6p, Pu 6d, and Pu 5f orbital, resulting in the occurrence of new band structure. The adsorption and dissociation of CO 2 molecule are obviously promoted by preferentially occupying adsorbed O atoms, therefore, a potential CO 2 protection mechanism for plutonium-based materials is that in CO 2 molecule there occurs complete dissociation of CO 2 → C + O + O, then the dissociated C atom combines with O atom from O 2 dissociation and produces CO, which will inhibit the O 2 from further oxidizing Pu surface, and slow down the corrosion rate of plutonium-based materials.
Type of Medium:
Online Resource
ISSN:
1674-1056
DOI:
10.1088/1674-1056/abc158
Language:
Unknown
Publisher:
IOP Publishing
Publication Date:
2021
detail.hit.zdb_id:
2412147-2
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