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Size Selectivity in Heterolanthanide Molecular Complexes with a Ditopic Ligand

Title: Size Selectivity in Heterolanthanide Molecular Complexes with a Ditopic Ligand
Authors: Bellucci, Luca; Fioravanti, Lorenzo; Armelao, Lidia; Bottaro, Gregorio; Marchetti, Fabio; Pineider, Francesco; Poneti, Giordano; Samaritani, Simona; Labella, Luca
Contributors: Bellucci, Luca; Fioravanti, Lorenzo; Armelao, Lidia; Bottaro, Gregorio; Marchetti, Fabio; Pineider, Francesco; Poneti, Giordano; Samaritani, Simona; Labella, Luca
Publisher Information: WILEY-V C H VERLAG GMBH
Publication Year: 2023
Collection: Padua Research Archive (IRIS - Università degli Studi di Padova)
Subject Terms: X-ray diffraction; hetero-lanthanides complexe; lanthanide; luminescence; magnetometry
Description: The similar reactivity of lanthanides generally leads to statistically populated polynuclear complexes, making the rational design of ordered hetero-lanthanide compounds extremely challenging. Here we report on the site selectivity in hetero-lanthanide tetranuclear complexes afforded by the relatively simple ditopic pyterpyNO ligand (4'-(4-pyridil)-2,2':6',2"-terpyridine N-oxide). The sequential room temperature reaction of RE2(tta)(6)(pyterpyNO)(2) (where RE=Y, (1); Eu, (2), Dy, (3) Htta=2-thenoyltrifluoroacetone) with La(tta)(3)dme (dme=dimethoxyethane) yielded Y2La2(tta)(12)(pyterpyNO)(2) (4), Dy2La2(tta)(12)(pyterpyNO)(2) (5) and Eu2La2(tta)(12)(pyterpyNO)(2) (6). Single crystals X-ray diffraction studies showed that 4, 5 and 6 are isostructural, featuring a tetranuclear structure with two different metal coordination sites with coordination numbers 8 (CN8) and 9 (CN9). The two smaller cations are mainly bridged by the O-donor atoms of the NO groups of two pyterpyNO ligands (CN8), while the larger lanthanum centres are bound by a terpyridine unit (CN9). Size selectivity has been studied with structural and magnetic studies in the solid state and through F-19 NMR and photoluminescence studies in solution, showing a direct dependence on the difference of ionic radii of the ions and yielding a 91 % selectivity for 4. Furthermore, F-19 NMR, X-ray and PL studies pointed out that the nature of the product is independent from the synthetic route for compound Eu2Y2(tta)(12)(pyterpyNO)(2) (7), keeping the ion selectivity also for a self-assembly reaction. Unexpectedly, these studies have evidenced that selectivity is not exclusively governed by electrostatic interactions related to size dimensions.
Document Type: article in journal/newspaper
File Description: ELETTRONICO
Language: English
Relation: info:eu-repo/semantics/altIdentifier/pmid/36200677; info:eu-repo/semantics/altIdentifier/wos/WOS:000890530300001; volume:29; issue:3; firstpage:e202202823; numberofpages:14; journal:CHEMISTRY-A EUROPEAN JOURNAL; https://hdl.handle.net/11577/3476089
DOI: 10.1002/chem.202202823
Availability: https://hdl.handle.net/11577/3476089; https://doi.org/10.1002/chem.202202823
Rights: info:eu-repo/semantics/openAccess ; license:Creative commons ; license uri:http://creativecommons.org/licenses/by/4.0/
Accession Number: edsbas.BECC4AC9
Database: BASE