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源自四酮型配体的四核[CuLn]配合物。

Tetranuclear [CuLn] complexes derived from a tetraketone-type ligand.

作者信息

Shiga Takuya, Miyamoto Haruka, Okamoto Yukiko, Oshio Hiroki, Mihara Nozomi, Nihei Masayuki

机构信息

Degree Programs in Pure and Applied Sciences, Graduate School of Science and Technology, University of Tsukuba, Tennodai 1-1-1, Tsukuba, Ibaraki 305-8571, Japan.

出版信息

Dalton Trans. 2023 Mar 28;52(13):3947-3953. doi: 10.1039/d2dt03892g.

DOI:10.1039/d2dt03892g
PMID:36779535
Abstract

A series of tetranuclear [CuLn] complexes, CuGd(L)(NO)(HO)·HO (1), CuTb(L)(NO)(HO) (2) and [CuDy(L)(NO)(HO)]·1.5(HO) (3), were synthesized by a one-pot reaction using a simple tetraketone-type ligand (HL = (3,5)-4,5-dihydroxy-3,5-octadiene-2,7-dione). X-ray structural analyses revealed that each complex has a planar tetranuclear core of [CuLn] (Ln = Gd, Tb, and Dy), in which the Ln ion is accommodated in the centre of a CuO metallocycle. A cryomagnetic study revealed that all complexes show intramolecular ferromagnetic interactions between Cu(II) and Ln(III) ions. The [CuGd] complex (1) has an = 5 spin ground state and shows a magneto-caloric effect with a maximum magnetic entropy change (-Δ) of 16.4 J kg K (5 T, 2.4 K). On the other hand, the [CuTb] complex (2) shows a slow magnetic relaxation behavior under a zero magnetic field. The analysis of an Arrhenius plot reveals that the effective energy barrier of spin reversal is 13.1 K. The [CuDy] complex (3) also shows a slow magnetic relaxation under 1300 Oe dc magnetic field with an effective energy barrier of 6.82 K.

摘要

通过使用一种简单的四酮型配体（HL = (3,5)-4,5-二羟基-3,5-辛二烯-2,7-二酮）的一锅法反应，合成了一系列四核[CuLn]配合物，即CuGd(L)(NO)(H₂O)·H₂O (1)、CuTb(L)(NO)(H₂O) (2) 和 [CuDy(L)(NO)(H₂O)]·1.5(H₂O) (3)。X射线结构分析表明，每个配合物都具有[CuLn]（Ln = Gd、Tb和Dy）的平面四核核心，其中Ln离子位于Cu₂O金属环的中心。低温磁性研究表明，所有配合物在Cu(II)和Ln(III)离子之间都表现出分子内铁磁相互作用。[CuGd]配合物(1)具有S = 5的自旋基态，并表现出磁热效应，最大磁熵变(-ΔSm)为16.4 J kg⁻¹ K⁻¹（5 T，2.4 K）。另一方面，[CuTb]配合物(2)在零磁场下表现出缓慢的磁弛豫行为。对阿伦尼乌斯图的分析表明，自旋反转的有效能垒为13.1 K。[CuDy]配合物(3)在1300 Oe直流磁场下也表现出缓慢的磁弛豫，有效能垒为6.82 K。

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