Hybrid inorganic-organic materials are an attractive area of research as they can exhibit a wide array of physical and chemical properties via synthetic design. In particular, there has been a surge of interest in coordination polymers showing intrinsic magnetic and conductive properties. Nevertheless, few materials have been constructed with S-based nodes and linkers while detailed studies have shown that moving from O-based linkers to less electronegative and more donating S-based linkers improves delocalization and allows for potential redox-tunability. The stones that block the way to multi-functional sulfur-containing coordination polymers are poor crystallinity of materials and the poor synthetic accessibility of thiolate linkers. To overcome these issues, my work focuses on development of suitable precursors: via ligand exchange with thiophenolate, the well-studied Fe4S4 cluster can be connected with 1,4-benzene-dithiolate to generate highly crystalline and soluble 1D-chains; by capping with dibutyl-tin groups, the difficult-to-isolate tetrathiafulvalene-2,3,6,7-tetrathiolate (TTFtt4-) linker was stabilized, and further efficient transmetallation leads to a series of conductive coordination polymers. The redox events of these building blocks are utilized for altering conductivity and energy storage in the resulting materials. In addition, more studies are carried out on the magnetic, thermal and optical properties of such delocalized sulfur metal-organic materials following installation of radical linkers.

Synthesis and characterization of multifunctional sulfur-based metal organic materials

ACS Fall 2021

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