1. Tailored Lewis Acid Sites for High-Temperature Supported Single-Molecule Magnetism
- Author
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Moritz Bernhardt, Maciej Damian Korzyński, Zachariah James Berkson, Fabrice Pointillart, Boris Le Guennic, Olivier Cador, Christophe Copéret, Eidgenössische Technische Hochschule - Swiss Federal Institute of Technology [Zürich] (ETH Zürich), Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), ETH Zurich Grant program [ETH-44 18-1], ETH Zurich Postdoctoral Fellowships program [FEL-23 19-1], ETH+ Project SynMatLab, ETH Career Seed Award, and ERC-CoG-MULTIPROSMM [725184]
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[CHIM]Chemical Sciences - Abstract
Generating or even retaining slow magnetic relaxationin surfaceimmobilized single-molecule magnets (SMMs) from promising molecularprecursors remains a great challenge. Illustrative examples are organolanthanidecompounds that show promising SMM properties in molecular systems,though surface immobilization generally diminishes their magneticperformance. Here, we show how tailored Lewis acidic Al-(III) siteson a silica surface enable generation of a material with SMM characteristicsvia chemisorption of (Cp-ttt)(2)DyCl ((Cp-ttt)(-) = 1,2,4-tri-(tert-butyl)-cyclopentadienide).Detailed studies of this system and its diamagnetic Y analogue indicatethat the interaction of the metal chloride with surface Al sites resultsin a change of the coordination sphere around the metal center inducingfor the dysprosium-containing material slow magnetic relaxation upto 51 K with hysteresis up to 8 K and an effective energy barrier(U (eff)) of 449 cm(-1),the highest reported thus far for a supported SMM., Journal of the American Chemical Society, 145 (23), ISSN:0002-7863, ISSN:1520-5126
- Published
- 2023
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