Effect of exchange-correlation functionals on the estimation of migration barriers in battery materials
Abstract Facile ionic mobility within host frameworks is crucial to the design of high-energy-density batteries with high-power-densities, where the migration barrier (E m ) is the governing factor. Here, we assess the accuracy and computational performance of generalized gradient approximation (GGA...
| Main Authors: | , , , |
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| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2022-07-01
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| Series: | npj Computational Materials |
| Online Access: | https://doi.org/10.1038/s41524-022-00837-0 |
| _version_ | 1817969601984593920 |
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| author | Reshma Devi Baltej Singh Pieremanuele Canepa Gopalakrishnan Sai Gautam |
| author_facet | Reshma Devi Baltej Singh Pieremanuele Canepa Gopalakrishnan Sai Gautam |
| author_sort | Reshma Devi |
| collection | DOAJ |
| description | Abstract Facile ionic mobility within host frameworks is crucial to the design of high-energy-density batteries with high-power-densities, where the migration barrier (E m ) is the governing factor. Here, we assess the accuracy and computational performance of generalized gradient approximation (GGA), the strongly constrained and appropriately normed (SCAN), and their Hubbard U corrections, GGA+U and SCAN+U, within the density functional theory-nudged elastic band framework, in the prediction of E m as benchmarked against experimental data. Importantly, we observe SCAN to be more accurate than other frameworks, on average, albeit with higher computational costs and convergence difficulties, while GGA is a feasible choice for “quick” and “qualitative” E m predictions. Further, we quantify the sensitivity of E m with adding uniform background charge and/or the climbing image approximation in solid electrolytes, and the Hubbard U correction in electrodes. Our findings will improve the quality of E m predictions which will enable identifying better materials for energy storage applications. |
| first_indexed | 2024-04-13T20:23:18Z |
| format | Article |
| id | doaj.art-c6c1a898bbdb4e0c8fd3ecc6175e1d2d |
| institution | Directory Open Access Journal |
| issn | 2057-3960 |
| language | English |
| last_indexed | 2024-04-13T20:23:18Z |
| publishDate | 2022-07-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | npj Computational Materials |
| spelling | doaj.art-c6c1a898bbdb4e0c8fd3ecc6175e1d2d2022-12-22T02:31:28ZengNature Portfolionpj Computational Materials2057-39602022-07-018111310.1038/s41524-022-00837-0Effect of exchange-correlation functionals on the estimation of migration barriers in battery materialsReshma Devi0Baltej Singh1Pieremanuele Canepa2Gopalakrishnan Sai Gautam3Department of Materials Engineering, Indian Institute of ScienceDepartment of Materials Science and Engineering, National University of SingaporeDepartment of Materials Science and Engineering, National University of SingaporeDepartment of Materials Engineering, Indian Institute of ScienceAbstract Facile ionic mobility within host frameworks is crucial to the design of high-energy-density batteries with high-power-densities, where the migration barrier (E m ) is the governing factor. Here, we assess the accuracy and computational performance of generalized gradient approximation (GGA), the strongly constrained and appropriately normed (SCAN), and their Hubbard U corrections, GGA+U and SCAN+U, within the density functional theory-nudged elastic band framework, in the prediction of E m as benchmarked against experimental data. Importantly, we observe SCAN to be more accurate than other frameworks, on average, albeit with higher computational costs and convergence difficulties, while GGA is a feasible choice for “quick” and “qualitative” E m predictions. Further, we quantify the sensitivity of E m with adding uniform background charge and/or the climbing image approximation in solid electrolytes, and the Hubbard U correction in electrodes. Our findings will improve the quality of E m predictions which will enable identifying better materials for energy storage applications.https://doi.org/10.1038/s41524-022-00837-0 |
| spellingShingle | Reshma Devi Baltej Singh Pieremanuele Canepa Gopalakrishnan Sai Gautam Effect of exchange-correlation functionals on the estimation of migration barriers in battery materials npj Computational Materials |
| title | Effect of exchange-correlation functionals on the estimation of migration barriers in battery materials |
| title_full | Effect of exchange-correlation functionals on the estimation of migration barriers in battery materials |
| title_fullStr | Effect of exchange-correlation functionals on the estimation of migration barriers in battery materials |
| title_full_unstemmed | Effect of exchange-correlation functionals on the estimation of migration barriers in battery materials |
| title_short | Effect of exchange-correlation functionals on the estimation of migration barriers in battery materials |
| title_sort | effect of exchange correlation functionals on the estimation of migration barriers in battery materials |
| url | https://doi.org/10.1038/s41524-022-00837-0 |
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