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Updated: Dec 27, 2025
Author Spotlight: Magnetometric Characterization of Intermediates in the Solid-State Electrochemistry of Redox-Active Metal-Organic Frameworks
Published on: June 9, 2023
Effects of Mixed Valency in an Fe-Based Framework: Coexistence of Slow Magnetic Relaxation, Semiconductivity, and
Ryuichi Murase1,2, Christopher J Commons2, Timothy A Hudson2
1School of Chemistry, The University of Sydney, Sydney, New South Wales 2006, Australia.
Abstract:
A 2-D coordination framework, (NEt4)2[Fe2(fan)3] (1·5(acetone); H2fan = 3,6-difluoro-2,5-dihydroxy-1,4-benzoquinone), was synthesized and structurally characterized. The compound is structurally analogous to a formerly elucidated framework, (NEt4)2[Fe2(can)3] (H2can = 3,6-dichloro-2,5-dihydroxy-1,4-benzoquinone), and adopts a 2-D (6,3) topology with the symmetrical stacking of [Fe2(fan)3]2- sheets that are held in position by the NEt4+ cations between the sheets. The investigation of the dc and ac magnetic properties of 1·5(acetone) revealed ferromagnetic ordering behavior and slow magnetization relaxation, as evinced from ac susceptibility measurements. Furthermore, the exposure of 1·5(acetone) to air led to the formation of a heptahydrate 1·7HO which displayed distinct magnetic properties. The study of the redox state and extent of delocalization in 1·5(acetone) was undertaken via crystallography, in combination with Mössbauer and vis-NIR spectroscopy, to reveal the mixed-valence and delocalized nature of the as-synthesized material. As a result, the conductivity studies conducted on a pressed pellet showed a relatively high conductivity of 1.8 × 10-2 S cm-1 (300 K). In order to compare structurally related anilate-based structures, a relationship among the redox state, spectroscopic properties, and electronic properties was elucidated in this work. A preliminary investigation of 1·5(acetone) as a candidate anode material in lithium ion batteries revealed a high reversible capacity of 676.6 mAh g-1 and high capacity retention.
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