Combining electron transfer, spin crossover, and redox properties in metal-organic frameworks

Livia Getzner, Damian Paliwoda, Laure Vendier, Latévi Max Lawson-Daku, Aurelian Rotaru, Gábor Molnár, Saioa Cobo () and Azzedine Bousseksou ()
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Livia Getzner: INP
Damian Paliwoda: INP
Laure Vendier: INP
Latévi Max Lawson-Daku: CH-1211 Genève 4
Aurelian Rotaru: Stefan cel Mare University of Suceava
Gábor Molnár: INP
Saioa Cobo: INP
Azzedine Bousseksou: INP

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: Abstract Hofmann coordination polymers (CPs) that couple the well-studied spin transition of the FeII central ion with electron-responsive ligands provide an innovative strategy toward multifunctional metal-organic frameworks (MOFs). Here, we developed a 2D planar network consisting of metal-cyanide-metal sheets in an unusual coordination mode, brought about by infinitely π-stacked redox-active bipyridinium derivatives as axial ligands. The obtained family of materials show vivid thermochromism attributed to electron transfer and/or electronic spin state change processes that can occur either independently or concomitantly. Importantly, the redox activity of the ligands within the structure leads to the quasi-reversible electrochemical reduction reaction on a spin-crossover complex at solid state. These observations have been confirmed via temperature-dependent single-crystal X-ray diffraction, magnetic measurements, Mössbauer, EPR, optical and vibrational spectroscopies as well as quantum chemical calculations.

Date: 2024
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DOI: 10.1038/s41467-024-51385-8

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