DFT + U and ab initio atomistic thermodynamics approache for mixed transitional metallic oxides

A case study of CoCu 2 O 3 surface terminations

Hantarto Widjaja, Hussein A. Miran, Mohammednoor Altarawneh, Ibukun Oluwoye, Hong Ngee Lim, Nay Ming Huang, Zhong Tao Jiang, Bogdan Z. Dlugogorski

Research output: Contribution to journalArticleResearchpeer-review

Abstract

This study develops a systematic density functional theory alongside on-site Coulomb interaction correction (DFT + U) and ab initio atomistic thermodynamics approachs for ternary (or mixed transitional metal oxides), expressed in three reservoirs. As a case study, among notable multiple metal oxides, synthesized CoCu 2 O 3 exhibits favourable properties towards applications in solar, thermal and catalytic processes. This progressive contribution applies DFT + U and atomistic thermodynamic approaches to examine the structure and relative stability of CoCu 2 O 3 surfaces. Twenty-five surfaces along the [001], [010], [100], [011], [101], [110] and [111] low-Miller-indices, with varying surface-termination configurations were selected in this study. The results portray satisfactory geometrical parameters for bulk CoCu 2 O 3 and a band gap of 1.25 e V. Furthermore, we clarified the stoichiometrically balanced inverted (010)CoCuO, and the non-stoichiometric (001)CuOCu, (001)CoOCo, (110)OCoO and (110)CoOCu surface terminations as the most stable configurations, out of which, the (001)CuOCu shows the optimum stability in ambient conditions. The systematic approach applied in this study should prove instrumental for the analysis of other 3-element multicomponent systems. To the best of our knowledge, the present study is the first to report DFT + U analysis to any 3-multicompnent systems with two of them requires inclusion of U treatment (i.e., f- and d- orbitals) in the electronic structure calculations.

Original languageEnglish
Pages (from-to)241-250
Number of pages10
JournalMaterials Chemistry and Physics
Volume201
Issue numberNovember
Early online date19 Aug 2017
DOIs
Publication statusPublished - 1 Nov 2017
Externally publishedYes

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Discrete Fourier transforms
Oxides
Thermodynamics
thermodynamics
oxides
metal oxides
Metals
mixed oxides
configurations
Coulomb interactions
Electronic structure
Density functional theory
Energy gap
inclusions
density functional theory
electronic structure
orbitals
interactions

Cite this

Widjaja, Hantarto ; Miran, Hussein A. ; Altarawneh, Mohammednoor ; Oluwoye, Ibukun ; Lim, Hong Ngee ; Huang, Nay Ming ; Jiang, Zhong Tao ; Dlugogorski, Bogdan Z. / DFT + U and ab initio atomistic thermodynamics approache for mixed transitional metallic oxides : A case study of CoCu 2 O 3 surface terminations. In: Materials Chemistry and Physics. 2017 ; Vol. 201, No. November. pp. 241-250.
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DFT + U and ab initio atomistic thermodynamics approache for mixed transitional metallic oxides : A case study of CoCu 2 O 3 surface terminations. / Widjaja, Hantarto; Miran, Hussein A.; Altarawneh, Mohammednoor; Oluwoye, Ibukun; Lim, Hong Ngee; Huang, Nay Ming; Jiang, Zhong Tao; Dlugogorski, Bogdan Z.

In: Materials Chemistry and Physics, Vol. 201, No. November, 01.11.2017, p. 241-250.

Research output: Contribution to journalArticleResearchpeer-review

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T1 - DFT + U and ab initio atomistic thermodynamics approache for mixed transitional metallic oxides

T2 - A case study of CoCu 2 O 3 surface terminations

AU - Widjaja, Hantarto

AU - Miran, Hussein A.

AU - Altarawneh, Mohammednoor

AU - Oluwoye, Ibukun

AU - Lim, Hong Ngee

AU - Huang, Nay Ming

AU - Jiang, Zhong Tao

AU - Dlugogorski, Bogdan Z.

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N2 - This study develops a systematic density functional theory alongside on-site Coulomb interaction correction (DFT + U) and ab initio atomistic thermodynamics approachs for ternary (or mixed transitional metal oxides), expressed in three reservoirs. As a case study, among notable multiple metal oxides, synthesized CoCu 2 O 3 exhibits favourable properties towards applications in solar, thermal and catalytic processes. This progressive contribution applies DFT + U and atomistic thermodynamic approaches to examine the structure and relative stability of CoCu 2 O 3 surfaces. Twenty-five surfaces along the [001], [010], [100], [011], [101], [110] and [111] low-Miller-indices, with varying surface-termination configurations were selected in this study. The results portray satisfactory geometrical parameters for bulk CoCu 2 O 3 and a band gap of 1.25 e V. Furthermore, we clarified the stoichiometrically balanced inverted (010)CoCuO, and the non-stoichiometric (001)CuOCu, (001)CoOCo, (110)OCoO and (110)CoOCu surface terminations as the most stable configurations, out of which, the (001)CuOCu shows the optimum stability in ambient conditions. The systematic approach applied in this study should prove instrumental for the analysis of other 3-element multicomponent systems. To the best of our knowledge, the present study is the first to report DFT + U analysis to any 3-multicompnent systems with two of them requires inclusion of U treatment (i.e., f- and d- orbitals) in the electronic structure calculations.

AB - This study develops a systematic density functional theory alongside on-site Coulomb interaction correction (DFT + U) and ab initio atomistic thermodynamics approachs for ternary (or mixed transitional metal oxides), expressed in three reservoirs. As a case study, among notable multiple metal oxides, synthesized CoCu 2 O 3 exhibits favourable properties towards applications in solar, thermal and catalytic processes. This progressive contribution applies DFT + U and atomistic thermodynamic approaches to examine the structure and relative stability of CoCu 2 O 3 surfaces. Twenty-five surfaces along the [001], [010], [100], [011], [101], [110] and [111] low-Miller-indices, with varying surface-termination configurations were selected in this study. The results portray satisfactory geometrical parameters for bulk CoCu 2 O 3 and a band gap of 1.25 e V. Furthermore, we clarified the stoichiometrically balanced inverted (010)CoCuO, and the non-stoichiometric (001)CuOCu, (001)CoOCo, (110)OCoO and (110)CoOCu surface terminations as the most stable configurations, out of which, the (001)CuOCu shows the optimum stability in ambient conditions. The systematic approach applied in this study should prove instrumental for the analysis of other 3-element multicomponent systems. To the best of our knowledge, the present study is the first to report DFT + U analysis to any 3-multicompnent systems with two of them requires inclusion of U treatment (i.e., f- and d- orbitals) in the electronic structure calculations.

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