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Supramolecular Tuning of Spin Crossover Properties in Isostructural Cocrystal Solvates

Lee T. Birchall, Amber T. Raja, Lewis Jackson, Helena J. Shepherd

2023Crystal Growth & Design20 citationsDOIOpen Access PDF

Abstract

High Resolution Image Download MS PowerPoint Slide In order to improve strategies for the design of spin-crossover materials, it is necessary to develop and understand structure–property relationships, and this is best achieved by obtaining isostructural materials. In this work we synthesized a series of four isostructural cocrystal solvates using the [Fe(3-bpp) 2 ][A] 2 complex and the 2,2-dipyridyl disulfide coformer in methanol and ethanol (A = BF 4 – or PF 6 – ). The spin-crossover properties of the materials were determined by variable temperature single-crystal X-ray diffraction. They show the same SCO behavior but with shifted spin-crossover temperatures, which has been related to the hydrogen bond basicity, p K BHX of the anions, and solvents present. This relationship between hydrogen bond basicity and the spin-crossover transition temperature offers a design strategy for the supramolecular tuning of spin-crossover properties in specific isostructural materials.

Topics & Concepts

IsostructuralSpin crossoverCocrystalSupramolecular chemistryHydrogen bondChemistryCrystallographyCrystal engineeringCrystal structureMaterials scienceMoleculeOrganic chemistryMagnetism in coordination complexesOrganic and Molecular Conductors ResearchMetal complexes synthesis and properties