The syntheses, structures and magnetic properties of the compounds of formula [FeIII(5-NO2sal2-trien)][MnIICrIII(ox)3]·CH3NO2·0.5H2O (1) and [FeIII(5-CH3Osal2-trien)][MnIICrIII(ox)3] (2) are reported. The structure of 1, that crystallizes in the P21 chiral space group, presents a 2D honeycomb anionic layer formed by MnII and CrIII ions linked through oxalate ligands and a cationic layer of [FeIII(5-NO2sal2-trien)]+ complexes intercalated between the 2D oxalate network. The structure of 2, that crystallizes in the Pna21 acentric space group, presents a 3D achiral anionic network formed by MnII and CrIII ions linked through oxalate ligands with [Fe(5-CH3Osal2-trien)]+ complexes intercalated within the 3D oxalate network. The magnetic properties of 1 and 2 indicate that both compounds undergo a long-range ferromagnetic ordering at ca. 5 K. On the other hand, the inserted FeIII cations remain mainly in the low-spin (LS) state in the case of 1 and in the high-spin (HS) state in the case of 2.
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