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双 TEMPO 配位的钆(III)、镧(III)和钇(III)配合物。稀土离子之间的强超交换耦合。

Doubly TEMPO-coordinated gadolinium(III), lanthanum(III), and yttrium(III) complexes. Strong superexchange coupling across rare earth ions.

机构信息

Department of Engineering Science, The University of Electro-Communications, Chofu, Tokyo 182-8585, Japan.

出版信息

Dalton Trans. 2014 Apr 21;43(15):5893-8. doi: 10.1039/c3dt53586j. Epub 2014 Mar 3.

DOI:10.1039/c3dt53586j
PMID:24589504
Abstract

We prepared crystalline [RE(III)(hfac)3(TEMPO)2] (RE = Gd, La, Y), where TEMPO and hfac stand for 2,2,6,6-tetramethylpiperidin-1-oxyl and 1,1,1,5,5,5-hexafluoropentane-2,4-dionate, respectively. The X-ray crystal structure of TEMPO-coordinated RE compounds was determined for the first time. The Gd and Y analogues are isomorphous, and the La derivative has a similar molecular skeleton. The Gd-O(TEMPO) bond lengths were 2.322(3) and 2.354(3) Å with the O-Gd-O angle of 140.36(11)°. The magnetic study clarified that [Gd(hfac)3(TEMPO)2] behaved as a ground Stotal = 7/2 species. The La and Y analogues showed the superexchange interactions across the diamagnetic ions with 2JTEMPO1-TEMPO2/kB = -14.9(1) and -49.8(2) K, respectively. Assuming the presence of a similar interaction like the Y derivative, the Gd-TEMPO exchange couplings are estimated with 2JGd-TEMPO/kB = -12.9(5) and +8.0(6) K.

摘要

我们制备了结晶态的[RE(III)(hfac)3(TEMPO)2]（RE = Gd、La、Y），其中 TEMPO 和 hfac 分别代表 2,2,6,6-四甲基哌啶-1-氧自由基和 1,1,1,5,5,5-六氟戊烷-2,4-二酮。首次确定了 TEMPO 配位的 RE 化合物的 X 射线晶体结构。Gd 和 Y 的类似物是同晶的，而 La 的衍生物具有相似的分子骨架。Gd-O(TEMPO)键长分别为 2.322(3)和 2.354(3)Å，O-Gd-O 角度为 140.36(11)°。磁性研究表明，[Gd(hfac)3(TEMPO)2]表现为基态总自旋 S = 7/2 物种。La 和 Y 的类似物表现出穿过反磁性离子的超交换相互作用，2JTEMPO1-TEMPO2/kB 分别为-14.9(1)和-49.8(2)K。假设存在类似于 Y 衍生物的类似相互作用，估计 Gd-TEMPO 交换耦合常数为 2JGd-TEMPO/kB = -12.9(5)和+8.0(6)K。

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