First-principles study of co-adsorption behavior of O2 and CO2 molecules on δ -Pu(100) surface

doi:10.1088/1674-1056/abc158

Abstract First principles calculation is performed to study the co-adsorption behaviors of O₂ and CO₂ 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-C₄O₇ and T_p1-C₂O₈, with adsorption energy of -17.296 eV and -23.131 eV for CO₂-based and O₂-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 CO₂ molecule are obviously promoted by preferentially occupying adsorbed O atoms, therefore, a potential CO₂ protection mechanism for plutonium-based materials is that in CO₂ molecule there occurs complete dissociation of CO

_{2} \to

C+O+O, then the dissociated C atom combines with O atom from O₂ dissociation and produces CO, which will inhibit the O₂ from further oxidizing Pu surface, and slow down the corrosion rate of plutonium-based materials.

Keywords: adsorption energy density functional theory electron density reaction mechanism

Received: 15 August 2020
Revised: 12 October 2020
Accepted manuscript online: 15 October 2020

PACS:	66.30.-h	(Diffusion in solids)
	65.40.gh	(Work functions)
	68.35.-p	(Solid surfaces and solid-solid interfaces: structure and energetics)
	71.15.Mb	(Density functional theory, local density approximation, gradient and other corrections)

Corresponding Authors: ^†Corresponding author. E-mail: wtao009@163.com

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Chun-Bao Qi(戚春保), Tao Wang(王涛), Ru-Song Li(李如松), Jin-Tao Wang(王金涛), Ming-Ao Qin(秦铭澳), and Si-Hao Tao(陶思昊) First-principles study of co-adsorption behavior of O₂ and CO₂ molecules on δ -Pu(100) surface 2021 Chin. Phys. B 30 026601

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First-principles study of co-adsorption behavior of O2 and CO2 molecules on δ -Pu(100) surface

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First-principles study of co-adsorption behavior of O₂ and CO₂ molecules on δ -Pu(100) surface