Advances in ab initio thermodynamic studies on metal/oxide interfaces

Abstract

We provide a brief overview of the advances in ab initio thermodynamic studies on metal/oxide interfaces in this paper. Firstly, the development in interface modeling is briefly outlined. Secondly, the fundamentals of ab initio thermodynamic method are described. Thirdly, ab initio thermodynamic studies on several typical interfaces between alumina and metals including alloys are presented, especially for the interfaces between α‐Al2O3 and Nb, Ni, Cu, and β‐Ni1−xAlx alloy. Finally, through analyzing electronic structure, chemical bonding, and adhesion of the interfaces between α‐Al2O3 and a series of metals, including Al, Ni, Cu, Au, Ag, Rh, Ir, Pd, Pt, Nb, and β‐NiAl, a formally unified model is derived for evaluating the works of separation of the representative aluminum‐rich, oxygen‐rich, and stoichiometric metal/α‐Al2O3 interfaces. This model is also expected to be valid for studying other metal/oxide interfaces.

First-Principles Study on the Effect of Pure and Oxidized Transition-Metal Buffers on Adhesion at the Alumina/Zinc Interface

“…This trend is consistent with the existing experimental evidence 1 and is corroborated by the results of ab initio calculations of metal adsorption on alumina films and surfaces. 20,22,29,43 Similar trends have also been reported for other non-reactive metal/oxide interfaces, such as, e.g., metal/MgO(100). 44,45 Results of the bond analysis along the series, Tab…”

“…9 The Al-terminated, non polar, stoichiometric basal (0001) plane , 17,18 the most stable surface in vacuum environment , 19 is a reference for the studies of metal-oxide interfaces. 1,[20][21][22][23][24] Despite a strong applicative interest and the widespread use of sapphire in the growth of epitaxial zinc oxide layers, 25 the nature of interactions and the adhesion strength at alumina/zinc interface have received only little attention in the past. [26][27][28][29] In a previous theoretical study we have shown that zinc adatoms interact weakly with the most stable, stoichiometric α-Al 2 O 3 (0001) surface, which is consistent with the poor wetting of anti-corrosive coatings.…”

“…In the present study, we focus on the α-Al 2 O 3 (0001) surface, which displays surface characteristics similar to those of more complex γ-alumina crystallites identified in model steel oxidation experiments or to those observed on industrial grades . The Al-terminated, nonpolar, stoichiometric basal (0001) plane, , the most stable surface in vacuum environment, is a reference for the studies of metal–oxide interfaces. ,− Despite a strong applicative interest and the widespread use of sapphire in the growth of epitaxial zinc oxide layers, the nature of interactions and the adhesion strength at alumina/zinc interface have received only little attention in the past. − In a previous theoretical study, we have shown that zinc adatoms interact weakly with the most stable, stoichiometric α-Al 2 O 3 (0001) surface, which is consistent with the poor wetting of anticorrosive coatings . An increase of bonding strength can only be induced by a net surface charge due to either surface polarity or an excess of surface hydroxyls.…”

Environment-dependent interfacial strength using first principles thermodynamics: The example of the Pt-HfO2 interface

“…10 On the computational side, first-principles density functional theory (DFT) computations have been instrumental in determining and understanding W sep for a plethora of important metal-insulator interfaces. [3][4][5][6][7][8][11][12][13][14][15][16][17][18][19][20][21][22][23][24][25] However, a major drawback of past DFT work is that they apply strictly to 0 K situations. Since the interface atomic configuration appropriate for a given set of experimental measurement conditions (temperature and pressure) is a priori not known, the general practice has been to compute W sep for a variety of different interfacial atomic configurations.…”

First principles calculations of solid–solid interfaces: an application to conversion materials for lithium-ion batteries

“…Their low thickness, possible reactivity and difficulty of access from bulk or surface techniques explain why only a few experimental works report data on solid/solid interfaces. Theoretical approaches are interesting tools [1][2][3][4] and have been successfully applied for example to the metal/ceramic interface and wetting [5][6][7] or to conversion materials for Li-ion batteries. [8][9][10] In these studies, periodic calculations at a Density Functional Theory (DFT) level are used in order to compute interface formation energies or works of adhesion and separation which could be compared, in a Yound-Dupr e formalism, to wetting experiments.…”