Multi-step spin-crossover in a 2D Hofmann-type clathrate with bisubstituted pyrazine†

IF 3.3 3区化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR

Dalton Transactions Pub Date : 2025-07-08 DOI:10.1039/D5DT01158B

Xiangkun Wen, Mengling Wu, Yancong Chen, Yanru Chen, Zhaoping Ni and Mingliang Tong

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Abstract

Multi-step spin-crossover (SCO) materials, which exhibit multiple distinct spin states, are considered promising candidates for high-order data storage and multiple switches. However, such materials remain rare, necessitating the development of innovative design strategies. Here, we chose an inexpensive asymmetric ligand, 2-chloro-6-methylpyrazine (ClMepz), and synthesized two-dimensional (2D) Hofmann-type clathrates [Fe(ClMepz)₂{M(CN)₂}₂]·ClMepz (M = Au (1), Ag (2)), in which ClMepz serves as a monodentate ligand and a guest molecule. Unlike the two-step SCO behavior in 2, compound 1 possesses more spin states and exhibits multi-step SCO behavior. The magneto-structural analysis reveals that the more linear [Au(CN)₂]⁻ unit exerts greater stress on the Hofmann layer, leading to the antiferro-elastic interactions. Additionally, the asymmetric host–guest interactions contribute to the stepwise SCO properties. Thus, the incorporation of asymmetric bisubstituted ligands into 2D Hofmann-type systems represents a viable and cost-effective strategy for the development of multi-step SCO materials.

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二维霍夫曼型双取代吡嗪包合物的多步自旋交叉

多步自旋交叉（SCO）材料具有多种不同的自旋状态，被认为是高阶数据存储和多开关的有前途的候选者。然而，这样的材料仍然很少，需要创新设计策略的发展。本文选择了一种廉价的不对称配体——2-氯-6-甲基吡嗪（ClMepz），合成了二维（2D） hofmann型包合物[Fe(ClMepz)2{M(CN)2}2]·ClMepz (M = Au (1), Ag(2))，其中ClMepz作为单齿配体和靶分子。与2中的两步SCO行为不同，配合物1具有更多的自旋态并表现出多步SCO行为。磁结构分析表明，越线性的[Au(CN)2]−单元对Hofmann层施加的应力越大，导致反铁-弹性相互作用。此外，不对称主客体相互作用有助于逐步SCO特性。因此，将不对称双取代配体结合到二维霍夫曼型体系中代表了开发多步SCO材料的可行且具有成本效益的策略。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Dalton Transactions 化学-无机化学与核化学

CiteScore

6.60

自引率

7.50%

发文量

1832

审稿时长

1.5 months

期刊介绍： Dalton Transactions is a journal for all areas of inorganic chemistry, which encompasses the organometallic, bioinorganic and materials chemistry of the elements, with applications including synthesis, catalysis, energy conversion/storage, electrical devices and medicine. Dalton Transactions welcomes high-quality, original submissions in all of these areas and more, where the advancement of knowledge in inorganic chemistry is significant.