Bimetallic complexes of the transition metals containing mixed diimine and dithiolate ligands are of fundamental interest on account of their intriguing electronic properties. Almost always, such complexes are isolated as species in which both the metal centers are in identical coordination environments - this means that the two metals often have identical redox properties. In contrast, mixed-diimine/dithiolate bimetallic complexes of the first row transition metals where the two metals are in dissimilar coordination environments are exceedingly rare, and are only known for nickel. Herein, we report the first ever example of a mixed-diimine/dithiolate dicobalt complex where the two cobalt centers are in different coordination environments. The synthesis of this compound is straightforward, and produces a complex in which the two cobalt centers display very different redox properties.

Unprecedented Inequivalent Metal Coordination Environments in a Mixed‐Ligand Dicobalt Complex

Synthesis, crystal structure and properties of electro-catalysis for hydrogen production of a molecular nickel catalyst based on bis(1,2,5-thiadiazole-3,4-dithiolate) ligand

Through theoretical calculations and magnetostructural study of nine radical compounds that exhibit strong anti-ferromagnetic coupling strength, it is revealed preliminarily that the overlap integral between adjacent radicals short contact atoms is relevant to associated strong anti-ferromagnetic coupling strength. It is also confirmed that spin density and overlap integral between adjacent radical short contact atoms are the two major factors that dominate intermolecular strong anti-ferromagnetic coupling strength. The study also reveals that the factor of the overlap integral can replace the factors of both interatomic short contact distance and slippage degrees of π-π stacking. The study also reveals for the first time that the overlap integral changes with different short contact atom and different central coordinated atom.

Study on adjacent radicals short contact interaction, spin density, overlap integral and strong anti-ferromagnetic coupling strength

A new ionic pair salt [Ni(bpy)(3)][Ni(mnt)(2)](2) (mnt = 1,2-dicyanoethane-1,2-dithiolate) has been prepared and its crystal structure was determined by X-ray crystallography at 293, 200 and 100 K. In the mononuclear radical anionic complex, the nickel ion assumes a slightly distorted square-planar geometry. There is a special kind of stacking interactions at each temperature (i.e., Model A at 293 K, Model B at 200 K and Model C at 100 K). The variable-temperature magnetic moments indicate that there is a strong anti-ferromagnetic interaction between the adjacent pi-pi stacking mononuclear mononuclear radical anionic complexes and especially the anti-ferromagnetic coupling strength is close to the diamagnetism at 100 K. The theoretical calculations reveal for the first time that the spin densities between the short contact atoms are beta state and the anti-ferromagnetic coupling property of this crystal may be related to the beta state spin densities between the short contact atoms. The theoretical calculations further confirm that the strong anti-ferromagnetic coupling strength should be relevant to the larger spin densities on the short contact atoms and the larger overlap integrals between the short contact atoms.

Intermolecular Magnetic Coupling Mechanism for a New Ionic Pair Salt [Ni(bpy)(3)][Ni(mnt)(2)](2)

Synthesis, crystal structures, and magnetism of the binuclear radical complex [N-methylpyridinium] 2 [Ni(tdas) 2 ] 2

Synthesis, crystal structure, and π–π stacking magnetism of the mononuclear radical complex [N-hydrogenpyridinium][Pd(mnt)2]

The binuclear radical complex [N-hydrogenpyridinium]2[Ni(tdas)2]2 (tdas = 1,2,5-thiazole-3,4-dithiolate) has been prepared and its crystal structure determined by X-ray crystallography. In the binuclear radical complex, the two nickel ions assume a distorted pyramidal geometry and are bridged by two sulfurs of different tdas anionic ligands. ESR spectra and the theoretical calculations reveal a very strong antiferromagnetic interaction in the binuclear radical complex, leading to diamagnetic crystals. The theoretical calculations also reveal a very weak antiferromagnetic interaction between adjacent radical complexes. This study is the first to report the magnetism of a binuclear radical nickel complex with tdas as ligand.

Synthesis, crystal structure, and magnetism of the binuclear radical complex [N-hydrogenpyridinium]2[Ni(tdas)2]2

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Synthesis, crystal structures, and magnetism of the binuclear radical complex [N-methylpyridinium] 2 [Ni(tdas) 2 ] 2

Synthesis, crystal structure, and π–π stacking magnetism of the mononuclear radical complex [N-hydrogenpyridinium][Pd(mnt)2]

Synthesis, crystal structure, and magnetism of the binuclear radical complex [N-hydrogenpyridinium]2[Ni(tdas)2]2