Influence of the synthesis and crystallization processes on the cation distribution in a series of multivariate rare-earth metal-organic frameworks and their magnetic characterization

Vasile, R. L. ; Godoy, A. A. ; Puente Orench, I. ; Nemes, N. M. ; Peña O''Shea, V. A. de la ; Gutiérrez-Puebla, E. ; Martínez, J. L. ; Monge, M. Á. ; Gándara, F.

Resumen: The incorporation of multiple metal atoms in multivariate metal-organic frameworks is typically carried out through a one-pot synthesis procedure that involves the simultaneous reaction of the selected elements with the organic linkers. In order to attain control over the distribution of the elements and to be able to produce materials with controllable metal combinations, it is required to understand the synthetic and crystallization processes. In this work, we have completed a study with the RPF-4 MOF family, which is made of various rare-earth elements, to investigate and determine how the different initial combinations of metal cations result in different atomic distributions in the obtained materials. Thus, we have found that for equimolar combinations involving lanthanum and another rare-earth element, such as ytterbium, gadolinium, or dysprosium, a compositional segregation takes place in the products, resulting in crystals with different compositions. On the contrary, binary combinations of ytterbium, gadolinium, erbium, and dysprosium result in homogeneous distributions. This dissimilar behavior is ascribed to differences in the crystallization pathways through which the MOF is formed. Along with the synthetic and crystallization study and considering the structural features of this MOF family, we also disclose here a comprehensive characterization of the magnetic properties of the compounds and the heat capacity behavior under different external magnetic fields.

Idioma: Inglés

DOI: 10.1021/acs.chemmater.2c01481

Año: 2022

Publicado en: Chemistry of materials 34, 15 (2022), 7029-7041
ISSN: 0897-4756

Factor impacto JCR: 8.6 (2022)

Categ. JCR: MATERIALS SCIENCE, MULTIDISCIPLINARY rank: 63 / 343 = 0.184 (2022) - Q1 - T1
Categ. JCR: CHEMISTRY, PHYSICAL rank: 38 / 161 = 0.236 (2022) - Q1 - T1

Factor impacto CITESCORE: 15.9 - Materials Science (Q1) - Chemistry (Q1) - Chemical Engineering (Q1)

Factor impacto SCIMAGO: 2.869 - Chemical Engineering (miscellaneous) (Q1) - Materials Chemistry (Q1) - Chemistry (miscellaneous) (Q1)

Financiación: info:eu-repo/grantAgreement/ES/AEI/CTQ2017-87262-R
Financiación: info:eu-repo/grantAgreement/ES/AEI/PID2019-107675RB-I00
Financiación: info:eu-repo/grantAgreement/ES/AEI/PID2021-122770B-I00
Financiación: info:eu-repo/grantAgreement/ES/MCIN/PLEC2021-007906
Financiación: info:eu-repo/grantAgreement/ES/MCIN/PRE2018-086059
Financiación: info:eu-repo/grantAgreement/ES/MINECO/PID2019--106315RB-I00

Tipo y forma: Artículo (Versión definitiva)