Evaluating structure selection in the hydrothermal growth of FeS₂ pyrite and marcasite
While the ab initio prediction of the properties of solids and their optimization towards new proposed materials is becoming established, little predictive theory exists as to which metastable materials can be made and how, impeding their experimental realization. Here we propose a quasi-thermodynam...
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| Other Authors: | |
| Format: | Article |
| Language: | en_US |
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Nature Publishing Group
2017
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| Online Access: | http://hdl.handle.net/1721.1/107628 https://orcid.org/0000-0003-2309-3644 |
| _version_ | 1826212907147329536 |
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| author | Kitchaev, Daniil Andreevich Ceder, Gerbrand |
| author2 | Massachusetts Institute of Technology. Department of Materials Science and Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Materials Science and Engineering Kitchaev, Daniil Andreevich Ceder, Gerbrand |
| author_sort | Kitchaev, Daniil Andreevich |
| collection | MIT |
| description | While the ab initio prediction of the properties of solids and their optimization towards new proposed materials is becoming established, little predictive theory exists as to which metastable materials can be made and how, impeding their experimental realization. Here we propose a quasi-thermodynamic framework for predicting the hydrothermal synthetic accessibility of metastable materials and apply this model to understanding the phase selection between the pyrite and marcasite polymorphs of FeS₂. We demonstrate that phase selection in this system can be explained by the surface stability of the two phases as a function of ambient pH within nano-size regimes relevant to nucleation. This result suggests that a first-principles understanding of nano-size phase stability in realistic synthesis environments can serve to explain or predict the synthetic accessibility of structural polymorphs, providing a guideline to experimental synthesis via efficient computational materials design. |
| first_indexed | 2024-09-23T15:40:22Z |
| format | Article |
| id | mit-1721.1/107628 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T15:40:22Z |
| publishDate | 2017 |
| publisher | Nature Publishing Group |
| record_format | dspace |
| spelling | mit-1721.1/1076282022-10-02T03:19:43Z Evaluating structure selection in the hydrothermal growth of FeS₂ pyrite and marcasite Kitchaev, Daniil Andreevich Ceder, Gerbrand Massachusetts Institute of Technology. Department of Materials Science and Engineering Kitchaev, Daniil Andreevich Ceder, Gerbrand While the ab initio prediction of the properties of solids and their optimization towards new proposed materials is becoming established, little predictive theory exists as to which metastable materials can be made and how, impeding their experimental realization. Here we propose a quasi-thermodynamic framework for predicting the hydrothermal synthetic accessibility of metastable materials and apply this model to understanding the phase selection between the pyrite and marcasite polymorphs of FeS₂. We demonstrate that phase selection in this system can be explained by the surface stability of the two phases as a function of ambient pH within nano-size regimes relevant to nucleation. This result suggests that a first-principles understanding of nano-size phase stability in realistic synthesis environments can serve to explain or predict the synthetic accessibility of structural polymorphs, providing a guideline to experimental synthesis via efficient computational materials design. National Science Foundation (U.S.) (Award No. OCI-1147503) National Energy Research Scientific Computing Center (U.S.) (contract no. DE-AC02-05CH11231) 2017-03-22T13:00:16Z 2017-03-22T13:00:16Z 2016-12 2016-03 Article http://purl.org/eprint/type/JournalArticle 2041-1723 http://hdl.handle.net/1721.1/107628 Kitchaev, Daniil A., and Gerbrand Ceder. “Evaluating Structure Selection in the Hydrothermal Growth of FeS2 Pyrite and Marcasite.” Nature Communications 7 (December 14, 2016): 13799. https://orcid.org/0000-0003-2309-3644 en_US http://dx.doi.org/10.1038/ncomms13799 Nature Communications Creative Commons Attribution 4.0 International License http://creativecommons.org/licenses/by/4.0/ application/pdf Nature Publishing Group Nature |
| spellingShingle | Kitchaev, Daniil Andreevich Ceder, Gerbrand Evaluating structure selection in the hydrothermal growth of FeS₂ pyrite and marcasite |
| title | Evaluating structure selection in the hydrothermal growth of FeS₂ pyrite and marcasite |
| title_full | Evaluating structure selection in the hydrothermal growth of FeS₂ pyrite and marcasite |
| title_fullStr | Evaluating structure selection in the hydrothermal growth of FeS₂ pyrite and marcasite |
| title_full_unstemmed | Evaluating structure selection in the hydrothermal growth of FeS₂ pyrite and marcasite |
| title_short | Evaluating structure selection in the hydrothermal growth of FeS₂ pyrite and marcasite |
| title_sort | evaluating structure selection in the hydrothermal growth of fes₂ pyrite and marcasite |
| url | http://hdl.handle.net/1721.1/107628 https://orcid.org/0000-0003-2309-3644 |
| work_keys_str_mv | AT kitchaevdaniilandreevich evaluatingstructureselectioninthehydrothermalgrowthoffes2pyriteandmarcasite AT cedergerbrand evaluatingstructureselectioninthehydrothermalgrowthoffes2pyriteandmarcasite |