Theoretical insights into the hydroxyl-promoted H2 releasing reaction after H2O splitting on Pu-oxide surfaces

Zhang, Le; Sun, Bin; Zhang, Qili; Liu, Haifeng; Song, Haifeng

doi:10.1016/j.jnucmat.2023.154642

Cited by 4 publications

(2 citation statements)

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“…, the difference between the Coulomb U and exchange J parameters, hereafter referred to as U ) value of 4 eV is selected for the 5f electrons of Pu and U, according to our previous calculations 29,30 and other computational experience. 21,22,31–36 According to experimental and theoretical calculations (DFT + U ), the ground states of Pu 2 O 3 and PuO 2 are set to antiferromagnetic states (AFM). 28,37 Correction of van der Waals forces between H, H 2 , and plutonium oxide matrix using DFT-D3 method.…”

Section: Methodsmentioning

confidence: 99%

Theoretical study on the hydrogen distribution and diffusion at the PuO₂/α-Pu₂O₃ interface

Huang,

Zhu,

Guo

et al. 2024

RSC Adv.

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Section: Methodsmentioning

confidence: 99%

Theoretical study on the hydrogen distribution and diffusion at the PuO₂/α-Pu₂O₃ interface

Huang,

Zhu,

Guo

et al. 2024

RSC Adv.

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“…Zhang's team conducted a series of studies on the differences between PuO 2 and Pu 2 O 3 in their interaction with hydrogen, revealing the micro-mechanisms underlying the differences in hydrogen inhibition efficiency between the two [17,18]. In Zhang's latest research, concerned about the issue of hydrogen molecules precipitated after water splitting on the surface of plutonium oxide [19]. Yu studied the adsorption and dissociation process of H 2 on the surface of PuO 2 (110) and found that H 2 exhibits weak adsorption on the surface of PuO 2 (110), but may dissociate to form H atoms under certain conditions.…”

Section: Introductionmentioning

confidence: 99%

The Adsorption Behavior of Hydrogen on the PuO2(111) Surface: A DFT+U Study

Huang,

Zhu,

2024

Coatings

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Based on density functional theory, a first-principles study of the adsorption behavior of hydrogen atoms on the PuO2(111) surface is carried out in this work. Models for three different surface morphologies of PuO2(111) are established. It is found that the surface with the outermost oxygen atom (sub outer Pu atom) morphology has the best stability. Based on this model, the adsorption energy, bader charge, and electronic density of the states of a hydrogen atom at different adsorption sites are calculated. Finally, we analyzed the process of hydrogen dissociation into hydrogen atoms on the surface using the cNEB method. The results indicate that the top position of the outermost oxygen atom and the bridge position of the second outermost plutonium atom are relatively stable adsorption configurations, where hydrogen atoms lose electrons and release heat, forming O-H bonds with oxygen atoms. The density of states of O-p orbital electrons will undergo significant changes, reflecting the hybridization of O-p and H-s orbital electrons, forming a stable bonding effect. The dissociation of hydrogen molecules into two hydrogen atoms adsorbed on the top of oxygen atoms requires crossing an energy barrier of 1.06 eV. The decrease in total energy indicates that hydrogen tends to exist on the PuO2(111) surface in a hydrogen atom state. The research results lay the foundation for theoretically exploring the hydrogenation corrosion mechanism of the PuO2(111) surface, providing theoretical support for exploring the corrosion aging of plutonium oxide, predicting the material properties of plutonium oxide under extreme and special environments.

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Water accelerates parabolic oxidation of Pu-Ga alloy: from mechanism to model

Zhang,

Sun,

Zhang

et al. 2024

Applied Surface Science

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Theoretical insights into the hydroxyl-promoted H2 releasing reaction after H2O splitting on Pu-oxide surfaces

Cited by 4 publications

References 40 publications

Theoretical study on the hydrogen distribution and diffusion at the PuO₂/α-Pu₂O₃ interface

Theoretical study on the hydrogen distribution and diffusion at the PuO₂/α-Pu₂O₃ interface

The Adsorption Behavior of Hydrogen on the PuO2(111) Surface: A DFT+U Study

Water accelerates parabolic oxidation of Pu-Ga alloy: from mechanism to model

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Theoretical insights into the hydroxyl-promoted H2 releasing reaction after H2O splitting on Pu-oxide surfaces

Cited by 4 publications

References 40 publications

Theoretical study on the hydrogen distribution and diffusion at the PuO2/α-Pu2O3 interface

Theoretical study on the hydrogen distribution and diffusion at the PuO2/α-Pu2O3 interface

The Adsorption Behavior of Hydrogen on the PuO2(111) Surface: A DFT+U Study

Water accelerates parabolic oxidation of Pu-Ga alloy: from mechanism to model

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Product

Resources

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Theoretical study on the hydrogen distribution and diffusion at the PuO₂/α-Pu₂O₃ interface

Theoretical study on the hydrogen distribution and diffusion at the PuO₂/α-Pu₂O₃ interface