Ab initio Defect Energetics in LaBO<sub>3</sub> Perovskite Solid Oxide Fuel Cell Materials

Lee, Yueh‐Lin; Morgan, Dane; Kleis, Jesper

doi:10.1149/1.3205837

Cited by 53 publications

(87 citation statements)

References 19 publications

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“…The calculated capture energy of the surface for a H 2 O molecule (−0.781 eV) undertaken during further analysis of the interaction forming a H 2 O molecule on the top of O with the surface showed a weak chemical adsorption. Here, the definition of the surface oxygen vacancy formation energy is as follows [ 34 ]:

where

and

are the energies of the LaNiO 3 (001) surface; with and without an oxygen vacancy, respectively.

is the result of considering spin polarization.…”

Section: Resultsmentioning

confidence: 99%

A First Principles Study of H2 Adsorption on LaNiO3(001) Surfaces

Pan

Chen

et al. 2017

Materials

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The adsorption of H2 on LaNiO3 was investigated using density functional theory (DFT) calculations. The adsorption sites, adsorption energy, and electronic structure of LaNiO3(001)/H2 systems were calculated and indicated through the calculated surface energy that the (001) surface was the most stable surface. By looking at optimized structure, adsorption energy and dissociation energy, we found that there were three types of adsorption on the surface. First, H2 molecules completely dissociate and then tend to bind with the O atoms, forming two –OH bonds. Second, H2 molecules partially dissociate with the H atoms bonding to the same O atom to form one H2O molecule. These two types are chemical adsorption modes; however, the physical adsorption of H2 molecules can also occur. When analyzing the electron structure of the H2O molecule formed by the partial dissociation of the H2 molecule and the surface O atom, we found that the interaction between H2O and the (001) surface was weaker, thus, H2O was easier to separate from the surface to create an O vacancy. On the (001) surface, a supercell was constructed to accurately study the most stable adsorption site. The results from analyses of the charge population; electron localization function; and density of the states indicated that the dissociated H and O atoms form a typical covalent bond and that the interaction between the H2 molecule and surface is mainly due to the overlap-hybridization among the H 1s, O 2s, and O 2p states. Therefore, the conductivity of LaNiO3(001)/H2 is stronger after adsorption and furthermore, the conductivity of the LaNiO3 surface is better than that of the LaFeO3 surface.

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where

and

are the energies of the LaNiO 3 (001) surface; with and without an oxygen vacancy, respectively.

is the result of considering spin polarization.…”

Section: Resultsmentioning

confidence: 99%

A First Principles Study of H2 Adsorption on LaNiO3(001) Surfaces

Pan

Chen

et al. 2017

Materials

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“…This oxygen chemical potential value was obtained using standard DFT thermochemical equations as documented in previous studies. [ 72,73 ] Briefly, the chemical potential is calculated by shifting the DFT‐calculated energy of an isolated O 2 molecule to account for finite temperature gas enthalpy and entropy effects using experimental tabulated data. The pressure dependence is included assuming O 2 behaves as an ideal gas.…”

Section: Methodsmentioning

confidence: 99%

“…Vibrational free energy corrections are included assuming a basic Einstein model following previous work. [ 72,73 ] Finally, following previous work and the convention set by the materials project, [ 68 ] the shift of the O 2 energy to correct for systematic errors of O 2 modeled with GGA‐PBE to correctly obtain oxide formation energies is applied to the solid phase energies during the stability analysis, rather than to the O 2 gas chemical potential.…”

Section: Methodsmentioning

confidence: 99%

Unconventional Highly Active and Stable Oxygen Reduction Catalysts Informed by Computational Design Strategies

Liu

Jacobs

et al. 2022

Advanced Energy Materials

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Discovering and engineering new materials with fast oxygen surface exchange kinetics and robust long‐term stability is essential for the large‐scale, economically viable commercialization of solid oxide fuel cell (SOFC) technology. The perovskite catalyst material BaFe0.125Co0.125Zr0.75O3 (BFCZ75), predicted to be promising from recent density functional theory (DFT) calculations and unconventional due to its extremely high Zr content and low electronic conductivity, exhibits oxygen reduction reaction surface exchange rates on par with Ba0.5Sr0.5Co0.8Fe0.2O3 (BSCF) and excellent stability at typical operating temperatures. New composite electrodes are engineered by integrating BFCZ75 with commercial electrode materials La1–xSrxMnO3 (LSM) and La1–xSrxCoyFe1–yO3 (LSCF) and achieve high performance as measured by low area specific resistance (ASR) values, with the LSCF/BFCZ75 ASR values comparable to top performing noncomposite electrode materials such as SrCo0.8Sc0.2O3–δ, BaNb0.05Fe0.95O3–δ and BaCo0.7Fe0.22Y0.08O3–δ. The use of BFCZ75 as a composite with LSCF achieving low ASR values shows that BFCZ75 is highly active and can easily integrate into existing SOFC material supply chains, lowering the barrier for potential commercial application of new electrode materials. Finally, these findings point to a broader unexplored class of perovskite materials with high fractions of redox inactive species (e.g., Zr, Nb, and Ta) that may unlock new pathways to realizing improved commercial SOFCs.

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“…The DFT + U approach was used to describe the localized 3d electronic states in Fe. In line with earlier work [19,20], we choose a Hubbard-U value of 4.0 eV for the Fe 3d states. Spin-polarized calculations have been applied throughout.…”

Section: Calculation Methods and Modelmentioning

confidence: 99%

Theoretical Study of Hydrogen on LaFeO3 (010) Surface Adsorption and Subsurface Diffusion

et al. 2018

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Based on density functional theory, this paper studies the adsorption and the subsurface occupation by H on LaFeO3 (010) surface and their corresponding transition states. As shown from the results, the best storage positions of hydrogen are on the O top position of the LaFeO3 (010) surface and the interstice near the oxygen of the subsurface. In addition, the position of surface Fe atom can also store hydrogen, but H atom prefers to adsorb on O atom first. Whether the H atom is adsorbed on O or Fe atom, it is easy diffuse to the nearby more stable O atom. However, the diffusion between the Fe atoms is difficult to occur. The main diffusion path of the H atom from the surface to the subsurface is the process of inward layer by layer around the O atom. With the fracture of the old H–O bond and the formation of the new H–O bond, the H is around O atom to constantly repeat the process of a hopping-rotational diffusion. H diffuses through the nearest neighbor position, which is more favorable than the direct diffusion.

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Ab initio Defect Energetics in LaBO₃ Perovskite Solid Oxide Fuel Cell Materials

Cited by 53 publications

References 19 publications

A First Principles Study of H2 Adsorption on LaNiO3(001) Surfaces

A First Principles Study of H2 Adsorption on LaNiO3(001) Surfaces

Unconventional Highly Active and Stable Oxygen Reduction Catalysts Informed by Computational Design Strategies

Theoretical Study of Hydrogen on LaFeO3 (010) Surface Adsorption and Subsurface Diffusion

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Ab initio Defect Energetics in LaBO3 Perovskite Solid Oxide Fuel Cell Materials

Cited by 53 publications

References 19 publications

A First Principles Study of H2 Adsorption on LaNiO3(001) Surfaces

A First Principles Study of H2 Adsorption on LaNiO3(001) Surfaces

Unconventional Highly Active and Stable Oxygen Reduction Catalysts Informed by Computational Design Strategies

Theoretical Study of Hydrogen on LaFeO3 (010) Surface Adsorption and Subsurface Diffusion

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Ab initio Defect Energetics in LaBO₃ Perovskite Solid Oxide Fuel Cell Materials