Abstract
The aim of the present work is to highlight the unique role of anilato-ligands, derivatives of the 2,5-dioxy-1,4-benzoquinone framework containing various substituents at the 3 and 6 positions (X = H, Cl, Br, I, CN, etc.), in engineering a great variety of new materials showing peculiar magnetic and/or conducting properties. Homoleptic anilato-based molecular building blocks and related materials will be discussed. Selected examples of such materials, spanning from graphene-related layered magnetic materials to intercalated supramolecular arrays, ferromagnetic 3D monometallic lanthanoid assemblies, multifunctional materials with coexistence of magnetic/conducting properties and/or chirality and multifunctional metal-organic frameworks (MOFs) will be discussed herein. The influence of (i) the electronic nature of the X substituents and (ii) intermolecular interactions i.e., H-Bonding, Halogen-Bonding, π-π stacking and dipolar interactions, on the physical properties of the resulting material will be also highlighted. A combined structural/physical properties analysis will be reported to provide an effective tool for designing novel anilate-based supramolecular architectures showing improved and/or novel physical properties. The role of the molecular approach in this context is pointed out as well, since it enables the chemical design of the molecular building blocks being suitable for self-assembly to form supramolecular structures with the desired interactions and physical properties.
Highlights
In the design of molecule-based magnets the choice of the interacting metal ions and the bridging ligand plays a key role in tuning the nature and magnitude of the magnetic interaction between the metal ions, especially when the bridge contains electronegative groups that may act as “adjusting screws
The ability of chlorocyananilate to. This family of anionic complexes are versatile precursors (i) for constructing 2D molecule-based Ferrimagnets with tunable ordering temperature as a function of the halogen electronegativity (Section 2.2); (ii) as magnetic components for building up multifunctional molecular materials based on BEDT-TTF organic donors-based conductivity carriers (Section 3.2), in analogy with the relevant class of [M(ox)3]3− tris-chelated complexes which have produced the first family of molecular paramagnetic superconductors [122,123,124]
It can be envisaged that the real challenge of anilate-based materials is due to their peculiar features: (i) easy to modify or functionalize by the conventional synthetic methods of organic and coordination chemistry, with no influence on their coordination modes (ii) easy to tune the magnetic exchange coupling between the coordinated metals by a simple change of the X substituent (X = H, F, Cl, Br, I, NO2, OH, CN, Me, Et, etc.) at the 3,6 positions of the anilato moiety; (iii) influence of the electronic nature of the X substituents on the intermolecular interactions and the physical properties of the resulting materials
Summary
The aim of the present work is to highlight the key role of anilates in engineering new materials with new or improved magnetic and/or conducting properties and new technological applications. Selected examples of para-/ferri-magnetic, spin-crossover and conducting/magnetic multifunctional materials based on transition metal complexes of anilato-derivatives, on varying the substituents at the 3,6 positions of the anilato moiety, will be discussed whose structural features or physical properties are peculiar and/or unusual with respect to analogous compounds reported in the literature up to now. Their most appealing technological applications will be reported
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