Abstract
AbstractA novel tetraoxolene‐bridged Fe two‐dimensional honeycomb layered compound, (NPr4)2[Fe2(Cl2An)3] ⋅2 (acetone)⋅H2O (1), where Cl2Ann−=2,5‐dichloro‐3,6‐dihydroxy‐1,4‐benzoquinonate and NPr4+=tetrapropylammonium cation, has been synthesized. 1 revealed a thermally induced valence tautomeric transition at T1/2=236 K (cooling)/237 K (heating) between Fem+ (m=2 or 3) and Cl2Ann− (n=2 or 3) that induced valence modulations between [FeIIHSFeIIIHS(Cl2An2−)2(Cl2An.3−)]2− at T>T1/2 and [FeIIIHSFeIIIHS(Cl2An2−)(Cl2An.3−)2]2− at T<T1/2. Even in a two‐dimensional network structure, the low‐temperature phase [FeIIIHSFeIIIHS(Cl2An2−)(Cl2An.3−)2]2− valence set can be regarded as a magnetic chain‐knit network, where ferrimagnetic Δ and Λ chains of [FeIIIHS(Cl2An.3−)]∞ are alternately linked by the diamagnetic Cl2An2−. This results in a slow magnetization behavior attributed to the structure acting as a single‐chain magnet at lower temperatures.
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