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Towards Predicting the Sequential Appearance of Zeolitic Imidazolate Frameworks Synthesized by Mechanochemistry

We use computational materials methods to study the sequential appearance of zinc-based zeolitic imidazolate frameworks (ZIFs) generated in the mechanochemical conversion process. We consider nine ZIF topologies, namely RHO, ANA, QTZ, SOD, KAT, DIA, NEB, CAG and GIS, combined with the two ligands 2-...

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Autores principales: Cherif, Mohamed, Zhang, Gaixia, Gao, Yang, Sun, Shuhui, Vidal, François
Formato: Online Artículo Texto
Lenguaje:English
Publicado: MDPI 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8954221/
https://www.ncbi.nlm.nih.gov/pubmed/35335309
http://dx.doi.org/10.3390/molecules27061946
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author Cherif, Mohamed
Zhang, Gaixia
Gao, Yang
Sun, Shuhui
Vidal, François
author_facet Cherif, Mohamed
Zhang, Gaixia
Gao, Yang
Sun, Shuhui
Vidal, François
author_sort Cherif, Mohamed
collection PubMed
description We use computational materials methods to study the sequential appearance of zinc-based zeolitic imidazolate frameworks (ZIFs) generated in the mechanochemical conversion process. We consider nine ZIF topologies, namely RHO, ANA, QTZ, SOD, KAT, DIA, NEB, CAG and GIS, combined with the two ligands 2-methylimidazolate and 2-ethylimidazolate. Of the 18 combinations obtained, only six (three for each ligand) were actually observed during the mechanosynthesis process. Energy and porosity calculations based on density functional theory, in combination with the Ostwald rule of stages, were found to be insufficient to distinguish the experimentally observed ZIFs. We then show, using classical molecular dynamics, that only ZIFs withstanding quasi-hydrostatic pressure P ≥ 0.3 GPa without being destroyed were observed in the laboratory. This finding, along with the requirement that successive ZIFs be generated with decreasing porosity and/or energy, provides heuristic rules for predicting the sequences of mechanically generated ZIFs for the two ligands considered.
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spelling pubmed-89542212022-03-26 Towards Predicting the Sequential Appearance of Zeolitic Imidazolate Frameworks Synthesized by Mechanochemistry Cherif, Mohamed Zhang, Gaixia Gao, Yang Sun, Shuhui Vidal, François Molecules Article We use computational materials methods to study the sequential appearance of zinc-based zeolitic imidazolate frameworks (ZIFs) generated in the mechanochemical conversion process. We consider nine ZIF topologies, namely RHO, ANA, QTZ, SOD, KAT, DIA, NEB, CAG and GIS, combined with the two ligands 2-methylimidazolate and 2-ethylimidazolate. Of the 18 combinations obtained, only six (three for each ligand) were actually observed during the mechanosynthesis process. Energy and porosity calculations based on density functional theory, in combination with the Ostwald rule of stages, were found to be insufficient to distinguish the experimentally observed ZIFs. We then show, using classical molecular dynamics, that only ZIFs withstanding quasi-hydrostatic pressure P ≥ 0.3 GPa without being destroyed were observed in the laboratory. This finding, along with the requirement that successive ZIFs be generated with decreasing porosity and/or energy, provides heuristic rules for predicting the sequences of mechanically generated ZIFs for the two ligands considered. MDPI 2022-03-17 /pmc/articles/PMC8954221/ /pubmed/35335309 http://dx.doi.org/10.3390/molecules27061946 Text en © 2022 by the authors. https://creativecommons.org/licenses/by/4.0/Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Article
Cherif, Mohamed
Zhang, Gaixia
Gao, Yang
Sun, Shuhui
Vidal, François
Towards Predicting the Sequential Appearance of Zeolitic Imidazolate Frameworks Synthesized by Mechanochemistry
title Towards Predicting the Sequential Appearance of Zeolitic Imidazolate Frameworks Synthesized by Mechanochemistry
title_full Towards Predicting the Sequential Appearance of Zeolitic Imidazolate Frameworks Synthesized by Mechanochemistry
title_fullStr Towards Predicting the Sequential Appearance of Zeolitic Imidazolate Frameworks Synthesized by Mechanochemistry
title_full_unstemmed Towards Predicting the Sequential Appearance of Zeolitic Imidazolate Frameworks Synthesized by Mechanochemistry
title_short Towards Predicting the Sequential Appearance of Zeolitic Imidazolate Frameworks Synthesized by Mechanochemistry
title_sort towards predicting the sequential appearance of zeolitic imidazolate frameworks synthesized by mechanochemistry
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8954221/
https://www.ncbi.nlm.nih.gov/pubmed/35335309
http://dx.doi.org/10.3390/molecules27061946
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