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Zusammenfassung

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.