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Chin. Phys. B, 2021, Vol. 30(2): 026601    DOI: 10.1088/1674-1056/abc158

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

Chun-Bao Qi(戚春保)1, Tao Wang(王涛)1,†, Ru-Song Li(李如松)2, Jin-Tao Wang(王金涛)1, Ming-Ao Qin(秦铭澳)1, and Si-Hao Tao(陶思昊)1
1 Xi'an Research Institute of High Technology, Xi'an 710025, China; 2 Xi'an Jiaotong University, Xi'an 710049, China
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) (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:   

Cite this article: 

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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