Integrating spin-dependent emission and dielectric switching in FeII catenated metal-organic frameworks

Xue-Ru Wu, Shu-Qi Wu (), Zhi-Kun Liu, Ming-Xing Chen, Jun Tao, Osamu Sato and Hui-Zhong Kou ()
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Xue-Ru Wu: Tsinghua University
Shu-Qi Wu: Kyushu University, 744 Motooka, Nishi-ku
Zhi-Kun Liu: School of Chemistry and Chemical Engineering, Liangxiang Campus, Beijing Institute of Technology
Ming-Xing Chen: College of Chemistry and Molecular Engineering, Peking University
Jun Tao: School of Chemistry and Chemical Engineering, Liangxiang Campus, Beijing Institute of Technology
Osamu Sato: Kyushu University, 744 Motooka, Nishi-ku
Hui-Zhong Kou: Tsinghua University

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Mechanically interlocked molecules (MIMs) including famous catenanes show switchable physical properties and attract continuous research interest due to their potential application in molecular devices. The advantages of using spin crossover (SCO) materials here are enormous, allowing for control through diverse stimuli and highly specific functions, and enabling the transfer of the internal dynamics of MIMs from solution to solid state, leading to macroscopic applications. Herein, we report the efficient self-assembly of catenated metal-organic frameworks (termed catena-MOFs) induced by stacking interactions, through the combination of rationally selected flexible and conjugated naphthalene diimide-based bis-pyridyl ligand (BPND), [MI(CN)2]− (M = Ag or Au) and Fe2+ in a one-step strategy. The obtained bimetallic Hofmann-type SCO-MOFs [FeII(BPND){Ag(CN)2}2]·3CHCl3 (1Ag) and [FeII(BPND{Au(CN)2}2]·2CHCl3·2H2O (1Au) possess a unique three-dimensional (3D) catena-MOF constructed from the polycatenation of two-dimensional (2D) layers with hxl topology. Both complexes undergo thermal- and light-induced SCO. Significantly, abnormal increases in the maximum emission intensity and dielectric constant can be detected simultaneously with the switching of spin states. This research opens up SCO-actuated bistable MIMs that afford dual functionality of coupled fluorescence emission and dielectricity.

Date: 2024
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DOI: 10.1038/s41467-024-48425-8

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