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Conducting Anilate-Based Mixed-Valence Fe(II)Fe(III) Coordination Polymer: Small-polaron Hopping Model for Oxalate-Type Fe(II)Fe(III) 2D Networks
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The mixed-valence FeIIFeIII 2D coordination polymer formulated as [TAG][FeIIFeIII(ClCNAn)3]·(solvate) 1 (TAG = tris(amino)-guanidinium, ClCNAn2− = chlorocyanoanilate dianionic ligand) crystallized in the polar trigonal space group P3. In the solid-state structure, determined both at 150 and at 10 K, anionic 2D honeycomb layers [FeIIFeIII(ClCNAn)3]− establish in the ab plane, with an intralayer metal−metal distance of 7.860 Å, alternating with cationic layers of TAG. The similar Fe−O distances suggest electron delocalization and an average oxidation state of +2.5 for each Fe center. The cation imposes its C3 symmetry to the structure and engages in intermolecular N−H···Cl hydrogen bonding with the ligand. Magnetic susceptibility characterization indicates magnetic ordering below 4 K and the presence of a hysteresis loop at 2 K with a coercive field of 60 Oe. Mössbauer measurements are in agreement with the existence of Fe(+2.5) ions at RT and statistic charge localization at 10 K. The compound shows semiconducting behavior with the in-plane conductivity of 2 × 10−3 S/cm, 3 orders of magnitude higher than the perpendicular one. A small-polaron hopping model has been applied to a series of oxalate-type FeIIFeIII 2D coordination polymers, providing a clear explanation on the much higher conductivity of the anilate-based systems than the oxalate ones.
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SAHADEVAN, Suchithra, ABHERVÉ, Alexandre, MONNI, Noemi, SÁENZ DE PIPAÓN, Cristina, GALAN-MASCAROS, José ramón, WAERENBORGH, João c., VIEIRA, Bruno j. c., AUBAN-SENZIER, Pascale, PILLET, Sébastien, BENDEIF, El-eulmi, ALEMANY I CAHNER, Pere, CANADELL, Enric, MERCURI, Maria laura, AVARVARI, Narcis. Conducting Anilate-Based Mixed-Valence Fe(II)Fe(III) Coordination Polymer: Small-polaron Hopping Model for Oxalate-Type Fe(II)Fe(III) 2D Networks. _Journal of the American Chemical Society_. 2018. Vol. 140, núm. 39, pàgs. 12611-12621. [consulta: 23 de gener de 2026]. ISSN: 0002-7863. [Disponible a: https://hdl.handle.net/2445/184290]