New Highly Charged Iron(III) Metal−Organic Cube Stabilized by a Bulky Amine
Author
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Cruz, Carlos
Author
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Vega Carvallo, Andrés Igor
Author
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Spodine, Evgenia
Author
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Escuer, Albert
Author
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Marco, José F.
Author
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Menéndez, Nieves
Author
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Venegas Yazigi, Diego
Author
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Paredes García, Verónica
Admission date
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2021-01-27T20:11:33Z
Available date
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2021-01-27T20:11:33Z
Publication date
dc.date.issued
2020
Cita de ítem
dc.identifier.citation
ACS Omega 2020, 5, 22238−22247
es_ES
Identifier
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10.1021/acsomega.0c02420
Identifier
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https://repositorio.uchile.cl/handle/2250/178376
Abstract
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In this work, we report a new octanuclear cluster based on FeIII and the ligand 1H-imidazole-4,5-dicarboxylic acid, [Et3NH](12)[Fe-8(IDC)(12)]center dot 10DMF center dot 13H(2)O (1), with a metal core containing eight Fe-III connected by only one type of organic ligand. A peak at 573 m/z in the mass spectra of the compound suggests the adduct species {[Fe-8(IDC)(12)]+8H}(4-). By X-ray photoelectron spectroscopy, the oxidation state of the iron cation was confirmed to be 3+, also identifying the presence of a quaternary nitrogen species, which act as a countercation of the anionic metal core [Fe-8(IDC)(12)](12-). Mossbauer spectra recorded at different temperatures show an isomer shift and quadrupole splitting parameters that confirm the existence of only Fe-III-HS in the structure of 1. X-ray analysis reveals that compound 1 crystallizes in the orthorhombic system space group Ibam, confirming a molecular cluster structure with an almost regular cube as geometry, with the Fe-III atoms located at the corners of the cube and connected by mu-1 kappa N-2,O:2 kappa N-2',O '''-IDC3- bridges. Additionally, the magnetic measurements reveal a weak antiferromagnetic coupling in the Fe-8(III) coordination cluster (J = -3.8 cm(-1)). To the best of our knowledge, 1 is the first member of the family of cubes assembled with 1H-imidazole-4,5-dicarboxylic acid and Fe-III cation, exhibiting high pH stability over a broad pH range, making it an ideal candidate for the design of supramolecular structures and metal-organic frameworks.
es_ES
Patrocinador
dc.description.sponsorship
Comision Nacional de Investigacion Cientifica y Tecnologica (CONICYT)
CONICYT FONDECYT
1170887
Proyecto Anillo CONICYT ACT
1404
CONICYT-FONDEQUIP/PPMS/EQM130086
CONICYT-FONDEQUIP/EQM140060
LIAM3-CNRS No1027
AFB180001
CEDENNA
Spanish Agencia Estatal de Investigacio'n (AEI)
RTI2018-095303-B-C51
Comunidad de Madrid
Agencia Estatal de Investigacion Espanola
PGC2018-095642-B-I00