RESUMEN
N-Type thermoelectrics typically consist of small molecule dopant+polymer host. Only a few polymer dopant+polymer host systems have been reported, and these have lower thermoelectric parameters. N-type polymers with high crystallinity and order are generally used for high-conductivity ( σ ${\sigma }$ ) organic conductors. Few n-type polymers with only short-range lamellar stacking for high-conductivity materials have been reported. Here, we describe an n-type short-range lamellar-stacked all-polymer thermoelectric system with highest σ ${\sigma }$ of 78â S-1 , power factor (PF) of 163â µW m-1 K-2 , and maximum Figure of merit (ZT) of 0.53 at room temperature with a dopant/host ratio of 75â wt%. The minor effect of polymer dopant on the molecular arrangement of conjugated polymer PDPIN at high ratios, high doping capability, high Seebeck coefficient (S) absolute values relative to σ ${\sigma }$ , and atypical decreased thermal conductivity ( κ ${\kappa }$ ) with increased doping ratio contribute to the promising performance.
RESUMEN
A novel n-type copolymer dopant polystyrene-poly(4-vinyl-N-hexylpyridinium fluoride) (PSpF) with fluoride anions is designed and synthesized by reversible addition-fragmentation chain transfer (RAFT) polymerization. This is thought to be the first polymeric fluoride dopant. Electrical conductivity of 4.2 S cm-1 and high power factor of 67 µW m-1 K-2 are achieved for PSpF-doped polymer films, with a corresponding decrease in thermal conductivity as the PSpF concentration is increased, giving the highest ZT of 0.1. An especially high electrical conductivity of 58 S cm-1 at 88 °C and outstanding thermal stability are recorded. Further, organic transistors of PSpF-doped thin films exhibit high electron mobility and Hall mobility of 0.86 and 1.70 cm2 V-1 s-1 , respectively. The results suggest that polystyrene-poly(vinylpyridinium) salt copolymers with fluoride anions are promising for high-performance n-type all-polymer thermoelectrics. This work provides a new way to realize organic thermoelectrics with high conductivity relative to the Seebeck coefficient, high power factor, thermal stability, and broad processing window.