High-Throughput Computational Screening of Perovskites for Thermochemical Water Splitting Applications (2024)

Emery, A. A., Saal, J. E., Kirklin, S., Hegde, V. I. (2016). High-Throughput Computational Screening of Perovskites for Thermochemical Water Splitting Applications. Chemistry of Materials, 28(16), 5621-5634. https://doi.org/10.1021/acs.chemmater.6b01182

Emery, Antoine A. ; Saal, James E. ; Kirklin, Scott et al. / High-Throughput Computational Screening of Perovskites for Thermochemical Water Splitting Applications. In: Chemistry of Materials. 2016 ; Vol. 28, No. 16. pp. 5621-5634.

@article{d868fa6fbb7d4184a6e480aafb23efa1,

title = "High-Throughput Computational Screening of Perovskites for Thermochemical Water Splitting Applications",

abstract = "The use of hydrogen as fuel is a promising avenue to aid in the reduction of greenhouse effect gases released in the atmosphere. In this work, we present a high-throughput density functional theory (HT-DFT) study of 5,329 cubic and distorted perovskite ABO3 compounds to screen for thermodynamically favorable two-step thermochemical water splitting (TWS) materials. From a data set of more than 11,000 calculations, we screened materials based on the following: (a) thermodynamic stability and (b) oxygen vacancy formation energy that allow favorable TWS. From our screening strategy, we identify 139 materials as potential new candidates for TWS application. Several of these compounds, such as CeCoO3 and BiVO3, have not been experimentally explored yet for TWS and present promising avenues for further research. We show that taking into consideration all phases present in the A-B-O ternary phase, as opposed to only calculating the formation energy of a compound, is crucial to assess correctly the stability of a compound as it reduces the number of potential candidates from 5,329 to 383. Finally, our large data set of compounds containing stabilites, oxidation states, and ionic sizes allowed us to revisit the structural maps for perovskites by showing stable and unstable compounds simultaneously.",

author = "Emery, {Antoine A.} and Saal, {James E.} and Scott Kirklin and Hegde, {Vinay I.} and Chris Wolverton",

note = "Publisher Copyright: {\textcopyright} 2016 American Chemical Society.",

year = "2016",

month = aug,

day = "23",

doi = "10.1021/acs.chemmater.6b01182",

language = "English (US)",

volume = "28",

pages = "5621--5634",

journal = "Chemistry of Materials",

issn = "0897-4756",

publisher = "American Chemical Society",

number = "16",

}

Emery, AA, Saal, JE, Kirklin, S, Hegde, VI 2016, 'High-Throughput Computational Screening of Perovskites for Thermochemical Water Splitting Applications', Chemistry of Materials, vol. 28, no. 16, pp. 5621-5634. https://doi.org/10.1021/acs.chemmater.6b01182

High-Throughput Computational Screening of Perovskites for Thermochemical Water Splitting Applications. / Emery, Antoine A.; Saal, James E.; Kirklin, Scott et al.
In: Chemistry of Materials, Vol. 28, No. 16, 23.08.2016, p. 5621-5634.

Research output: Contribution to journal › Article › peer-review

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T1 - High-Throughput Computational Screening of Perovskites for Thermochemical Water Splitting Applications

AU - Emery, Antoine A.

AU - Saal, James E.

AU - Kirklin, Scott

AU - Hegde, Vinay I.

AU - Wolverton, Chris

N1 - Publisher Copyright:© 2016 American Chemical Society.

PY - 2016/8/23

Y1 - 2016/8/23

N2 - The use of hydrogen as fuel is a promising avenue to aid in the reduction of greenhouse effect gases released in the atmosphere. In this work, we present a high-throughput density functional theory (HT-DFT) study of 5,329 cubic and distorted perovskite ABO3 compounds to screen for thermodynamically favorable two-step thermochemical water splitting (TWS) materials. From a data set of more than 11,000 calculations, we screened materials based on the following: (a) thermodynamic stability and (b) oxygen vacancy formation energy that allow favorable TWS. From our screening strategy, we identify 139 materials as potential new candidates for TWS application. Several of these compounds, such as CeCoO3 and BiVO3, have not been experimentally explored yet for TWS and present promising avenues for further research. We show that taking into consideration all phases present in the A-B-O ternary phase, as opposed to only calculating the formation energy of a compound, is crucial to assess correctly the stability of a compound as it reduces the number of potential candidates from 5,329 to 383. Finally, our large data set of compounds containing stabilites, oxidation states, and ionic sizes allowed us to revisit the structural maps for perovskites by showing stable and unstable compounds simultaneously.

AB - The use of hydrogen as fuel is a promising avenue to aid in the reduction of greenhouse effect gases released in the atmosphere. In this work, we present a high-throughput density functional theory (HT-DFT) study of 5,329 cubic and distorted perovskite ABO3 compounds to screen for thermodynamically favorable two-step thermochemical water splitting (TWS) materials. From a data set of more than 11,000 calculations, we screened materials based on the following: (a) thermodynamic stability and (b) oxygen vacancy formation energy that allow favorable TWS. From our screening strategy, we identify 139 materials as potential new candidates for TWS application. Several of these compounds, such as CeCoO3 and BiVO3, have not been experimentally explored yet for TWS and present promising avenues for further research. We show that taking into consideration all phases present in the A-B-O ternary phase, as opposed to only calculating the formation energy of a compound, is crucial to assess correctly the stability of a compound as it reduces the number of potential candidates from 5,329 to 383. Finally, our large data set of compounds containing stabilites, oxidation states, and ionic sizes allowed us to revisit the structural maps for perovskites by showing stable and unstable compounds simultaneously.

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Emery AA, Saal JE, Kirklin S, Hegde VI, Wolverton C. High-Throughput Computational Screening of Perovskites for Thermochemical Water Splitting Applications. Chemistry of Materials. 2016 Aug 23;28(16):5621-5634. doi: 10.1021/acs.chemmater.6b01182