Early-Stage Formation of the SIFSIX-3-Zn Metal-Organic Framework: An Automated Computational Study.
Inorg Chem
; 62(3): 1210-1217, 2023 Jan 23.
Article
en En
| MEDLINE
| ID: mdl-36626658
ABSTRACT
Metal-organic frameworks (MOFs) have attracted significant attention over the past 2 decades due to their wide applicability as functional materials. However, targeted synthesis of novel MOFs remains problematic as their formation mechanisms are poorly understood, which forces us to rely on serendipity in the synthesis of novel MOFs. Here, we demonstrate a workflow employing the artificial force induced reaction (AFIR) method to investigate the self-assembly process of the node of the SIFSIX-3-Zn MOF, [Zn(pyz)4(SiF6)2]2- (pyz = pyrazine), in an automated manner. The workflow encompassing AFIR calculations, generation of extensive reaction path networks, propagation simulations of intermediates, and further refinements of identified formation pathways showed that the nodal structure can form through multiple competing pathways involving interconvertible intermediates. This finding provides a plausible rationale for the stochastic multistage processes believed to be key in MOF formation. Furthermore, this work represents the first application of an automated reaction mechanism discovery method to a MOF system using a general workflow that is applicable to study the formation of other MOF motifs as well.
Texto completo:
1
Colección:
01-internacional
Banco de datos:
MEDLINE
Asunto principal:
Estructuras Metalorgánicas
Tipo de estudio:
Prognostic_studies
Idioma:
En
Revista:
Inorg Chem
Año:
2023
Tipo del documento:
Article
País de afiliación:
Japón