Tailored Lewis Acid Sites for High-Temperature Supported Single-Molecule Magnetism,Journal of the American Chemical Society

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Tailored Lewis Acid Sites for High-Temperature Supported Single-Molecule Magnetism
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-06-01 , DOI: 10.1021/jacs.3c02730
Moritz Bernhardt ₁ , Maciej D Korzyński ₁ , Zachariah J Berkson ₁ , Fabrice Pointillart ₂ , Boris Le Guennic ₂ , Olivier Cador ₂ , Christophe Copéret ₁

Affiliation

Generating or even retaining slow magnetic relaxation in surface immobilized single-molecule magnets (SMMs) from promising molecular precursors remains a great challenge. Illustrative examples are organolanthanide compounds that show promising SMM properties in molecular systems, though surface immobilization generally diminishes their magnetic performance. Here, we show how tailored Lewis acidic Al(III) sites on a silica surface enable generation of a material with SMM characteristics via chemisorption of (Cp^ttt)₂DyCl ((Cp^ttt)⁻ = 1,2,4-tri(tert-butyl)-cyclopentadienide). Detailed studies of this system and its diamagnetic Y analogue indicate that the interaction of the metal chloride with surface Al sites results in a change of the coordination sphere around the metal center inducing for the dysprosium-containing material slow magnetic relaxation up to 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.

中文翻译：

用于高温支持的单分子磁性的定制路易斯酸位点

从有前途的分子前体在表面固定的单分子磁体 (SMM) 中产生甚至保持缓慢的磁弛豫仍然是一个巨大的挑战。说明性的例子是有机镧系化合物，它们在分子系统中显示出有前途的 SMM 特性，尽管表面固定化通常会降低它们的磁性能。在这里，我们展示了如何通过 (Cp ^ttt ) ₂ DyCl ((Cp ^ttt ) ⁻ = 1,2,4-tri( tert-丁基）-环戊二烯化物）。对该系统及其反磁性 Y 类似物的详细研究表明，金属氯化物与表面铝位点的相互作用导致金属中心周围的配位球发生变化，从而导致含镝材料的磁弛豫缓慢至 51 K，并具有滞后现象高达 8 K 和449 cm ^{–1的有效能垒 (}U _eff ) ，这是迄今为止报告的支持 SMM 的最高值。

更新日期：2023-06-01

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