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Accuracy of DFT computed oxygen-vacancy formation energies and high-throughput search of solar thermochemical water-splitting compounds
Abstract
The enthalpy change involved in metal oxide reduction is a key quantity in various processes related to energy conversion and storage, and is of particular interest for computational prediction. Often this prediction involves the simulation of a high temperature reduction process with a 0K methodology like density functional theory (DFT), and it is not infrequent for the high temperature and 0K stable crystal structures to differ. This introduces a conundrum with regards to the choice of crystal structure to utilize in the computation, with approaches in the literature varying and experimental validation remaining scarce. In this work we address both the crystal structure conundrum and the experimental validation, and then apply the insights we gain to guide a high-throughput search for new materials for solar thermochemical water-splitting applications. By computing the DFT+U oxygen vacancy formation energy (ΔEvf) of a selection of ABO3 compounds and comparing different crystal structures for each composition, we highlight the issues that arise when the structure utilized in the computation is dynamically unstable at 0K, namely the presence of an artificial lowering of ΔEvf, and the lack of convergence of ΔEvf with cell size. We solve these limitations by identifying and employing a suitable surrogate dynamicallymore »
- Authors:
-
[1];
[2];
[3];
[4];
[1];
[1];
[1]
- Northwestern University, Evanston, IL (United States)
- Northwestern University, Evanston, IL (United States); University of Science and Technology Beijing (China)
- Northwestern University, Evanston, IL (United States); Saint-Gobain Research North America, Northborough, MA (United States)
- Northwestern University, Evanston, IL (United States); University of Messina (Italy)
- Publication Date:
- Research Org.:
- Northwestern Univ., Evanston, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Energy Research Scientific Computing Center (NERSC)
- OSTI Identifier:
- 1984937
- Alternate Identifier(s):
- OSTI ID: 1985152
- Grant/Contract Number:
- EE0008089; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review Materials
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 6; Journal ID: ISSN 2475-9953
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 08 HYDROGEN; Energy applications; First-principles calculations; Hydrogen energy
Citation Formats
Baldassarri, Bianca, He, Jiangang, Qian, Xin, Mastronardo, Emanuela, Griesemer, Sean, Haile, Sossina M., and Wolverton, Christopher. Accuracy of DFT computed oxygen-vacancy formation energies and high-throughput search of solar thermochemical water-splitting compounds. United States: N. p., 2023.
Web. doi:10.1103/physrevmaterials.7.065403.
Baldassarri, Bianca, He, Jiangang, Qian, Xin, Mastronardo, Emanuela, Griesemer, Sean, Haile, Sossina M., & Wolverton, Christopher. Accuracy of DFT computed oxygen-vacancy formation energies and high-throughput search of solar thermochemical water-splitting compounds. United States. https://doi.org/10.1103/physrevmaterials.7.065403
Baldassarri, Bianca, He, Jiangang, Qian, Xin, Mastronardo, Emanuela, Griesemer, Sean, Haile, Sossina M., and Wolverton, Christopher. Wed .
"Accuracy of DFT computed oxygen-vacancy formation energies and high-throughput search of solar thermochemical water-splitting compounds". United States. https://doi.org/10.1103/physrevmaterials.7.065403.
@article{osti_1984937,
title = {Accuracy of DFT computed oxygen-vacancy formation energies and high-throughput search of solar thermochemical water-splitting compounds},
author = {Baldassarri, Bianca and He, Jiangang and Qian, Xin and Mastronardo, Emanuela and Griesemer, Sean and Haile, Sossina M. and Wolverton, Christopher},
abstractNote = {The enthalpy change involved in metal oxide reduction is a key quantity in various processes related to energy conversion and storage, and is of particular interest for computational prediction. Often this prediction involves the simulation of a high temperature reduction process with a 0K methodology like density functional theory (DFT), and it is not infrequent for the high temperature and 0K stable crystal structures to differ. This introduces a conundrum with regards to the choice of crystal structure to utilize in the computation, with approaches in the literature varying and experimental validation remaining scarce. In this work we address both the crystal structure conundrum and the experimental validation, and then apply the insights we gain to guide a high-throughput search for new materials for solar thermochemical water-splitting applications. By computing the DFT+U oxygen vacancy formation energy (ΔEvf) of a selection of ABO3 compounds and comparing different crystal structures for each composition, we highlight the issues that arise when the structure utilized in the computation is dynamically unstable at 0K, namely the presence of an artificial lowering of ΔEvf, and the lack of convergence of ΔEvf with cell size. We solve these limitations by identifying and employing a suitable surrogate dynamically stable structure. We then validate the predictive power of our calculations against appositely generated experimental measurements of reduction enthalpy for a series of Hubbard U values, finding an accuracy ranging between 0.2-0.6 eV/O. In light of such conclusions, we revise and expand a previous a high-throughput DFT study on ABO3 perovskite oxides. As a result, we provide a list of candidate STCH materials, highlight trends with redox-active cation and structural distortion, and identify Mn4+, Mn3+ and Co3+ as the most promising redox-active cations.},
doi = {10.1103/physrevmaterials.7.065403},
journal = {Physical Review Materials},
number = 6,
volume = 7,
place = {United States},
year = {Wed Jun 07 00:00:00 EDT 2023},
month = {Wed Jun 07 00:00:00 EDT 2023}
}
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