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    Rights statement: This is the author’s version of a work that was accepted for publication in Journal of Nuclear Materials. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Journal of Nuclear Materials, 482, 2016 DOI: 10.1016/j.jnucmat.2016.10.005

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Electronic structure of bulk AnO2 (An = U, Np, Pu) and water adsorption on the (111) and (110) surfaces of UO2 and PuO2 from hybrid density functional theory within the periodic electrostatic embedded cluster method

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Electronic structure of bulk AnO2 (An = U, Np, Pu) and water adsorption on the (111) and (110) surfaces of UO2 and PuO2 from hybrid density functional theory within the periodic electrostatic embedded cluster method. / Wellington, Joseph P. W.; Kerridge, Andrew; Austin, Jonathan; Kaltsoyannis, Nikolas.

In: Journal of Nuclear Materials, Vol. 482, 15.12.2016, p. 124-134.

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@article{855d32f4765241859eeaf708d9a642f1,
title = "Electronic structure of bulk AnO2 (An = U, Np, Pu) and water adsorption on the (111) and (110) surfaces of UO2 and PuO2 from hybrid density functional theory within the periodic electrostatic embedded cluster method",
abstract = "Generalised gradient approximation (PBE) and hybrid (PBE0) density functional theory (DFT) within the periodic electrostatic embedded cluster method have been used to study AnO2 bulk and surfaces (An = U, Np, Pu). The electronic structure has been investigated by examining the projected density of states (PDOS). While PBE incorrectly predicts these systems to be metallic, PBE0 finds them to be insulators, with the composition of the valence and conduction levels agreeing well with experiment. Molecular and dissociative water adsorption on the (111) and (110) surfaces of UO2 and PuO2 has been investigated, with that on the (110) surface being stronger than on the (111). Similar energies are found for molecular and dissociative adsorption on the (111) surfaces, while on the (110) there is a clear preference for dissociative adsorption. Adsorption energies and geometries on the (111) surface of UO2 are in good agreement with recent periodic DFT studies using the GGA+U approach, and our data for dissociative adsorption on the (110) surface of PuO2 match experiment rather well, especially when dispersion corrections are included.",
author = "Wellington, {Joseph P. W.} and Andrew Kerridge and Jonathan Austin and Nikolas Kaltsoyannis",
note = "This is the author’s version of a work that was accepted for publication in Journal of Nuclear Materials. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Journal of Nuclear Materials, 482, 2016 DOI: 10.1016/j.jnucmat.2016.10.005",
year = "2016",
month = "12",
day = "15",
doi = "10.1016/j.jnucmat.2016.10.005",
language = "English",
volume = "482",
pages = "124--134",
journal = "Journal of Nuclear Materials",
issn = "0022-3115",
publisher = "Elsevier Science B.V.",

}

RIS

TY - JOUR

T1 - Electronic structure of bulk AnO2 (An = U, Np, Pu) and water adsorption on the (111) and (110) surfaces of UO2 and PuO2 from hybrid density functional theory within the periodic electrostatic embedded cluster method

AU - Wellington, Joseph P. W.

AU - Kerridge, Andrew

AU - Austin, Jonathan

AU - Kaltsoyannis, Nikolas

N1 - This is the author’s version of a work that was accepted for publication in Journal of Nuclear Materials. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Journal of Nuclear Materials, 482, 2016 DOI: 10.1016/j.jnucmat.2016.10.005

PY - 2016/12/15

Y1 - 2016/12/15

N2 - Generalised gradient approximation (PBE) and hybrid (PBE0) density functional theory (DFT) within the periodic electrostatic embedded cluster method have been used to study AnO2 bulk and surfaces (An = U, Np, Pu). The electronic structure has been investigated by examining the projected density of states (PDOS). While PBE incorrectly predicts these systems to be metallic, PBE0 finds them to be insulators, with the composition of the valence and conduction levels agreeing well with experiment. Molecular and dissociative water adsorption on the (111) and (110) surfaces of UO2 and PuO2 has been investigated, with that on the (110) surface being stronger than on the (111). Similar energies are found for molecular and dissociative adsorption on the (111) surfaces, while on the (110) there is a clear preference for dissociative adsorption. Adsorption energies and geometries on the (111) surface of UO2 are in good agreement with recent periodic DFT studies using the GGA+U approach, and our data for dissociative adsorption on the (110) surface of PuO2 match experiment rather well, especially when dispersion corrections are included.

AB - Generalised gradient approximation (PBE) and hybrid (PBE0) density functional theory (DFT) within the periodic electrostatic embedded cluster method have been used to study AnO2 bulk and surfaces (An = U, Np, Pu). The electronic structure has been investigated by examining the projected density of states (PDOS). While PBE incorrectly predicts these systems to be metallic, PBE0 finds them to be insulators, with the composition of the valence and conduction levels agreeing well with experiment. Molecular and dissociative water adsorption on the (111) and (110) surfaces of UO2 and PuO2 has been investigated, with that on the (110) surface being stronger than on the (111). Similar energies are found for molecular and dissociative adsorption on the (111) surfaces, while on the (110) there is a clear preference for dissociative adsorption. Adsorption energies and geometries on the (111) surface of UO2 are in good agreement with recent periodic DFT studies using the GGA+U approach, and our data for dissociative adsorption on the (110) surface of PuO2 match experiment rather well, especially when dispersion corrections are included.

U2 - 10.1016/j.jnucmat.2016.10.005

DO - 10.1016/j.jnucmat.2016.10.005

M3 - Journal article

VL - 482

SP - 124

EP - 134

JO - Journal of Nuclear Materials

JF - Journal of Nuclear Materials

SN - 0022-3115

ER -