A new three-dimensional (3-D) jungle-gym-like open metal-organic framework has been synthesized from a two-dimensional (2-D) layer compound using a heterogeneous pillar insertion reaction. Both the starting 2-D layer and the resulting 3-D open compounds have been characterized using X-ray crystallography.
This study provides conclusive proof that the thermally excited open-shell state with biradical character is contributing to the ground state of a closed-shell molecule, tF-BDPI-2Y, where four hydrogen atoms at the central phenylene ring are substituted with four fluorine atoms of 1,4-bis-(4,5-diphenylimidazol-2-ylidene)cyclohexa-2,5-diene (BDPI-2Y). A small increase in the population of biradical species of tF-BDPI-2Y results in the formation of the dimer form by the radical recombination reaction. Controlling the equilibrium between a closed-shell diamagnetic-quinoid state and an open-shell paramagnetic-biradical state will provide significant progress in the field of π-conjugated delocalized biradical chemistry.
The novel complex trans-Cu(hfac)2(TTF-py)2 (hfac = hexafluoroacetylacetonate; TTF-py = 4-(2-tetrathiafulvalenyl-ethenyl)pyridine) in which the paramagnetic transition metal and the organic donor are covalently linked through a conjugated bridge is synthesized and characterized aiming at a new approach for the occurrence of π−d interactions in conducting and magnetic molecule-based materials.
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