A priori control of zeolite phase competition and intergrowth with high-throughput simulations
Zeolites are versatile catalysts and molecular sieves with large topological diversity, but managing phase competition in zeolite synthesis is an empirical, labor-intensive task. Here, we controlled phase selectivity in templated zeolite synthesis from first principles by combining high-throughput a...
| Main Authors: | , , , , , , , , , , |
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| Format: | Article |
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American Association for the Advancement of Science (AAAS)
2021
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| Online Access: | https://hdl.handle.net/1721.1/132618 |
| _version_ | 1811002140170125312 |
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| author | Schwalbe-Koda, Daniel Kwon, Soonhyoung Paris, Cecilia Bello-Jurado, Estefania Jensen, Zach Olivetti, Elsa A. Willhammar, Tom Corma, Avelino Román- Leshkov, Yuriy Moliner, Manuel Gómez-Bombarelli, Rafael |
| author2 | Massachusetts Institute of Technology. Department of Materials Science and Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Materials Science and Engineering Schwalbe-Koda, Daniel Kwon, Soonhyoung Paris, Cecilia Bello-Jurado, Estefania Jensen, Zach Olivetti, Elsa A. Willhammar, Tom Corma, Avelino Román- Leshkov, Yuriy Moliner, Manuel Gómez-Bombarelli, Rafael |
| author_sort | Schwalbe-Koda, Daniel |
| collection | MIT |
| description | Zeolites are versatile catalysts and molecular sieves with large topological diversity, but managing phase competition in zeolite synthesis is an empirical, labor-intensive task. Here, we controlled phase selectivity in templated zeolite synthesis from first principles by combining high-throughput atomistic simulations, literature mining, human-computer interaction, synthesis, and characterization. Proposed binding metrics distilled from over 586,000 zeolite-molecule simulations reproduced the extracted literature and rationalize framework competition in the design of organic structure-directing agents. Energetic, geometric, and electrostatic descriptors of template molecules were found to regulate synthetic accessibility windows and aluminum distributions in pure-phase zeolites. Furthermore, these parameters allowed realizing an intergrowth zeolite through a single bi-selective template. The computation-first approach enabled controlling both zeolite synthesis and structure composition using a priori theoretical descriptors. |
| first_indexed | 2024-09-23T15:43:48Z |
| format | Article |
| id | mit-1721.1/132618 |
| institution | Massachusetts Institute of Technology |
| last_indexed | 2024-09-23T15:43:48Z |
| publishDate | 2021 |
| publisher | American Association for the Advancement of Science (AAAS) |
| record_format | dspace |
| spelling | mit-1721.1/1326182022-09-29T15:48:12Z A priori control of zeolite phase competition and intergrowth with high-throughput simulations Schwalbe-Koda, Daniel Kwon, Soonhyoung Paris, Cecilia Bello-Jurado, Estefania Jensen, Zach Olivetti, Elsa A. Willhammar, Tom Corma, Avelino Román- Leshkov, Yuriy Moliner, Manuel Gómez-Bombarelli, Rafael Massachusetts Institute of Technology. Department of Materials Science and Engineering Massachusetts Institute of Technology. Department of Chemical Engineering Massachusetts Institute of Technology. Institute for Data, Systems, and Society Zeolites are versatile catalysts and molecular sieves with large topological diversity, but managing phase competition in zeolite synthesis is an empirical, labor-intensive task. Here, we controlled phase selectivity in templated zeolite synthesis from first principles by combining high-throughput atomistic simulations, literature mining, human-computer interaction, synthesis, and characterization. Proposed binding metrics distilled from over 586,000 zeolite-molecule simulations reproduced the extracted literature and rationalize framework competition in the design of organic structure-directing agents. Energetic, geometric, and electrostatic descriptors of template molecules were found to regulate synthetic accessibility windows and aluminum distributions in pure-phase zeolites. Furthermore, these parameters allowed realizing an intergrowth zeolite through a single bi-selective template. The computation-first approach enabled controlling both zeolite synthesis and structure composition using a priori theoretical descriptors. National Science Foundation (Awards 1922311, 1922372 and 1922090) Office of Naval Research (Contract N00014-20-1-2280) 2021-09-21T19:27:58Z 2021-09-21T19:27:58Z 2021-09 2021-03 Article http://purl.org/eprint/type/JournalArticle 0036-8075 1095-9203 https://hdl.handle.net/1721.1/132618 Schwalbe-Koda, Daniel et al. "A priori control of zeolite phase competition and intergrowth with high-throughput simulations." Science (September 2021): 10.1126/science.abh3350. © American Association for the Advancement of Science. http://dx.doi.org/10.1126/science.abh3350 Science Creative Commons Attribution-Noncommercial-Share Alike http://creativecommons.org/licenses/by-nc-sa/4.0/ application/pdf American Association for the Advancement of Science (AAAS) Prof. Rafael Gomez-Bombarelli via Ye Li |
| spellingShingle | Schwalbe-Koda, Daniel Kwon, Soonhyoung Paris, Cecilia Bello-Jurado, Estefania Jensen, Zach Olivetti, Elsa A. Willhammar, Tom Corma, Avelino Román- Leshkov, Yuriy Moliner, Manuel Gómez-Bombarelli, Rafael A priori control of zeolite phase competition and intergrowth with high-throughput simulations |
| title | A priori control of zeolite phase competition and intergrowth with high-throughput simulations |
| title_full | A priori control of zeolite phase competition and intergrowth with high-throughput simulations |
| title_fullStr | A priori control of zeolite phase competition and intergrowth with high-throughput simulations |
| title_full_unstemmed | A priori control of zeolite phase competition and intergrowth with high-throughput simulations |
| title_short | A priori control of zeolite phase competition and intergrowth with high-throughput simulations |
| title_sort | priori control of zeolite phase competition and intergrowth with high throughput simulations |
| url | https://hdl.handle.net/1721.1/132618 |
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