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Abstract:
This study introduces a novel synthetic strategy to modulate the electronic band structure of conjugated coordination polymers (c-CPs) through control of the redox state of hydroquinone/benzoquinone ligands during synthesis. We successfully synthesized two distinct semiconducting c-CPs, Ag4TTBQ(TTBQ=1,2,4,5-tetrathiolbenzoquinone) and Ag4TTHQ(TTHQ=1,2,4,5-tetrathiolhydroquinone), by reacting TTHQ with silver nitrate and silver acetate, respectively. Despite sharing the same topological structure, charge transport measurements and DFT calculations reveal significant differences in their electronic structures. Notably, Ag4TTHQ demonstrates superior thermoelectric performance compared to other silver-based c-CPs. This research unveils a pioneering approach to finely tune the electronic band structure and properties of c-CPs, and paves the way for advanced applications in high-performance thermoelectric and electronic devices.
