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Through Space π-Electrons Communication in [2,2]-Paracyclophanes: Unprecendented Stabilization of Radicals.
Angew Chem Int Ed Engl
December 2024
Institut Chimie radicalaire ICR-UMR 7273, Facult� de Saint jerome, avenue Escadrille-Normandie-Niemen, service 562, 13397, Marseille, FRANCE.
Efforts to understand radical stability have led to considerable progress in radical chemistry. In this article, we investigated a novel approach to enhancing the radical stability of carbon-centered radicals through space electron delocalization within [2,2]-paracyclophanes. Alkoxyamines possessing a paracyclophane scaffold exploit face-to-face π-π-interactions between the aromatic rings to effectively lower bond dissociation energy (BDE) for NO-C bond homolysis.
View Article and Find Full Text PDFSlow magnetic relaxation and strong magnetic coupling in the nitroxyl radical complexes of lanthanide(iii) with diamagnetic ground state (Ln = Lu, Eu).
Chem Sci
December 2024
Nikolayev Institute of Inorganic Chemistry, Siberian Branch, Russian Academy of Sciences 630090 Novosibirsk Russia
Radical lanthanide complexes are appealing platforms to investigate the possibility to engineer relevant magnetic couplings between the two magnetic centers by exploiting the strongly donating magnetic orbitals of the radical. In this paper, we report a spectroscopic and magnetic study on [LnRad(NO)], where Ln = Eu or Lu and Rad is the tridentate tripodal nitroxyl radical 4,4-dimethyl-2,2-bis(pyridin-2-yl)-1,3-oxazolidine-3-oxyl. A thorough magnetic investigation by Electron Paramagnetic Resonance (EPR) spectroscopy and magnetometry, fully supported by calculations, allowed us to unravel an unprecedentedly large antiferromagnetic coupling between the Eu and the radical ( = +19.
View Article and Find Full Text PDFSingle-Molecule Magnet Behavior in a Tb-Nitronyl Nitroxide Radical Network with [Tb(NIT)] Nodes.
Inorg Chem
December 2024
Laboratoire de Chimie de Coordination du CNRS (LCC-CNRS), Université de Toulouse, CNRS, Toulouse 31062, France.
Two rare two-dimensional Ln-radical networks, namely, [{Ln(tfa)}(NIT-4Py)] [Ln = Gd and Tb ; tfa = trifluoroacetylacetonato; and NIT-4Py = 2-(4-pyridyl)-4,4,5,5-tetramethylimidazoline-1-oxyl-3-oxide], have been successfully constructed and characterized. In these complexes, each NIT-4Py radical functions as a tridentate ligand to ligate three Ln ions, creating a 2D network with linear five-spin [Ln(NIT)] nodes. Ferromagnetic Ln-NO interactions govern the characteristic magnetic behavior of a finite spin system.
View Article and Find Full Text PDFRotaxane-catalyzed aerobic oxidation of primary alcohols.
Commun Chem
November 2024
Department of Chemistry "Giacomo Ciamician", University of Bologna, Via P. Gobetti 85, I-40129, Bologna, Italy.
Article Synopsis
- Nitroxide radicals serve as effective catalysts for oxidizing primary alcohols within a specially designed rotaxane structure that includes a paramagnetic crown ether and a molecular axle.
- The rotaxane's primary catalyst is a nitroxide radical that changes its oxidation state during the reaction, while Cerium(IV)/O acts as the co-oxidant.
- The study not only details the synthesis and characterization of the rotaxane using various analytical techniques but also explores its potential for developing autonomous molecular machines based on this catalytic process.
Light-induced spin-state switching in heterospin complexes of Cu(hfac) with pyridine-based nitroxides.
Dalton Trans
November 2024
International Tomography Center SB RAS, Novosibirsk, 630090, Russia.
Article Synopsis
- Copper(II)-nitroxide molecular magnets can switch spin states like spin-crossover, but understanding their properties remains difficult, especially for light-induced changes.
- This study investigates the photoswitching and relaxation of Cu(hfac)L complexes with pyridine-based ligands using electron paramagnetic resonance (EPR) methods.
- Results show long-lasting photoinduced spin states at low temperatures, but the effectiveness of switching is influenced by the size of the radical ligands, providing insights into the underlying mechanisms for these molecular magnets.
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