Journal
ADVANCED FUNCTIONAL MATERIALS
Volume 33, Issue 23, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202213911
Keywords
electrical conductivity; n-doping; organic thermoelectric; polymer semiconductors; selenium substitutions
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By devising a novel selenophene-based electron-deficient building block, the pronounced advantages of selenium substitution in enabling advanced n-type polymers are demonstrated. The resulting selenium-substituted polymer achieves high conductivity and power factor, surpassing the sulfur-based analogue polymer by 40% conductivity increase. These results provide important insights for developing high-performing n-type organic thermoelectric materials.
Designing n-type polymers with high electrical conductivity remains a major challenge for organic thermoelectrics (OTEs). Herein, by devising a novel selenophene-based electron-deficient building block, the pronounced advantages of selenium substitution in simultaneously enabling advanced n-type polymers is demonstrated with high mobility (approximate to 2 orders of magnitude higher versus their sulfur-based analogues due to both intensified intra- and inter-chain interactions) and much improved n-doping efficiency (enabled by the largely lowered LUMO level with a approximate to 0.2 eV margin) of the resulting polymers. Via side chain optimization and donor engineering, the selenium-substituted polymer, f-BSeI2TEG-FT, achieves a highest conductivity of 103.5 S cm(-1) and power factor of 70.1 mu W m(-1) K-2, which are among the highest values reported in literature for n-type polymers, and f-BSeI2TEG-FT greatly outperformed the sulfur-based analogue polymer by 40% conductivity increase. These results demonstrate that selenium substitution is a very effective strategy for improving n-type performance and provide important structure-property correlations for developing high-performing n-type OTE materials.
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