Synthesis, Crystal Structure and Properties of Iron Bisdicyanamide (Fe[N(CN)2]2) and Iron Diammin Bisdicyanamide (Fe[NH3]2[N(CN)2]2)

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Phase-pure iron bisdicyanamide (Fe(dca)2) forms a rutile-like 3D network that exhibits a ferrimagnetic transition at 19.1 K with long-range cooperative magnetic ordering, while its diammin derivative forms a layered monoclinic structure. Novelty: ClaimNovelty.INCREMENTAL. Consensus alignment: ConsensusAlignment.NEUTRAL.

Laura Henrich; Aylin Koldemir; Jan Hempelmann; Jan van Leusen; Rainer Pöttgen; Andreas Houben; Richard Dronskowski; Egbert Figgemeier

doi:10.3390/inorganics14080218

August 20, 2026InorganicsOpen Access

Synthesis, Crystal Structure and Properties of Iron Bisdicyanamide (Fe[N(CN)2]2) and Iron Diammin Bisdicyanamide (Fe[NH3]2[N(CN)2]2)

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Key Points

Synthesize phase-pure iron bisdicyanamide and iron diammin bisdicyanamide complexes to characterize their structural and magnetic behaviors.
Synthesized phase-pure Fe(dca)2 and Fe(dca)2(NH3)2 complexes.
Determined crystal structures across temperatures from 300 K down to 25 K and verified bonding via ATR-IR spectroscopy.
Characterized magnetic and thermal properties using SQUID magnetometry, Mößbauer spectroscopy, low-temperature neutron diffraction, and thermogravimetric analysis.
Fe(dca)2 adopts an orthorhombic Pnnm space group with a 3D rutile-like network, exhibiting a unit cell volume contraction of ~2.5 Å³ from 300 K to 25 K.
Fe(dca)2(NH3)2 crystallizes in the monoclinic P21/c space group as 2D layers coordinated by axial ammonia ligands.
Fe(dca)2 demonstrates a ferrimagnetic phase transition at TC = 19.1 K and displays magnetic hysteresis at 5 K.

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Implication

Experimental study reveals a 3D network with ferrimagnetic ordering at 19.1 K in iron bisdicyanamide, indicating robust long-range cooperative magnetic coupling.

Abstract

The phase-pure syntheses of Fe(dca)2 and Fe(dca)2(NH3)2 have enabled comprehensive investigation of their structural and magnetic properties. Fe(dca)2 crystallizes in the orthorhombic space group Pnnm, with Fe2+ ions octahedrally coordinated by six dca ligands, forming a rutile-like 3D network. Temperature-dependent structural analysis reveals minor distortions and a slight unit cell volume contraction (~2.5 Å3) from 300 K to 25 K. Fe(dca)2(NH3)2 crystallizes in the monoclinic space group P21/c, featuring two axial ammonia ligands and dca-bridged Fe2+ ions forming layers. Magnetic susceptibility measurements of Fe(dca)2 reveal a ferrimagnetic transition at TC = 19.1 K, confirmed by SQUID data, Mößbauer spectroscopic measurements and low-temperature neutron diffraction. A magnetic hysteresis at 5 K indicates long-range cooperative magnetic ordering. ATR-IR spectroscopic measurements support the structural models and confirm the chemical composition of both compounds. TGA shows the thermal decomposition of Fe(dca)2.

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Henrich et al. (2026) studied this question.

synapsesocial.com/papers/6a89600eca7ade938187f1b1 https://doi.org/10.3390/inorganics14080218

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Synthesis, Crystal Structure and Properties of Iron Bisdicyanamide (Fe[N(CN)2]2) and Iron Diammin Bisdicyanamide (Fe[NH3]2[N(CN)2]2)

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Cite This Study

Synthesis, Crystal Structure and Properties of Iron Bisdicyanamide (Fe[N(CN)2]2) and Iron Diammin Bisdicyanamide (Fe[NH3]2[N(CN)2]2)

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