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Inne
A 3D MOF based on adamantoid tetracopper(II) and aminophosphine oxide cages: structural features and magnetic and catalytic properties.
Autorzy
Rok wydania
2021
Czasopismo
Numer woluminu
60
Strony
9631-9644
DOI
10.1021/acs.inorgchem.1c00868
Kolekcja
Język
Angielski
Typ publikacji
Artykuł
This work describes an unexpected generation of a new 3D metal–organic framework (MOF), [Cu4(μ-Cl)6(μ4-O)Cu(OH)2(μ-PTA═O)4]n·2nCl-EtOH·2.5nH2O, from copper(II) chloride and 1,3,5-triaza-7-phosphaadamantane 7-oxide (PTA═O). The obtained product is composed of diamandoid tetracopper(II) [Cu4(μ-Cl)6(μ4-O)] cages and monocopper(II) [Cu(OH)2] units that are assembled, via the diamandoid μ-PTA═O linkers, into an intricate 3D net with an nbo topology. Magnetic susceptibility measurements on this MOF in the temperature range of 1.8–300 K reveal a ferromagnetic interaction (J = +20 cm–1) between the neighboring copper(II) ions. Single-point DFT calculations disclose a strong delocalization of the spin density over the tetranuclear unit. The magnitude of exchange coupling, predicted from the broken-symmetry DFT studies, is in good agreement with the experimental data. This copper(II) compound also acts as an active catalyst for the mild oxidation and carboxylation of alkanes. The present study provides a unique example of an MOF that is assembled from two different types of adamantoid Cu4 and PTA═O cages, thus contributing to widening a diversity of functional metal–organic frameworks.
Adres publiczny
http://dx.doi.org/10.1021/acs.inorgchem.1c00868
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