Lactone Backbone Density in Rigid Electron-Deficient Semiconducting Polymers Enabling High n-type Organic Thermoelectric Performance

Maryam Alsufyani*, Marc Antoine Stoeckel, Xingxing Chen, Karl Thorley, Rawad K. Hallani, Yuttapoom Puttisong, Xudong Ji, Dilara Meli, Bryan D. Paulsen, Joseph Strzalka, Khrystyna Regeta, Craig Combe, Hu Chen, Junfu Tian, Jonathan Rivnay, Simone Fabiano, Iain McCulloch

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

4 Scopus citations

Abstract

Three lactone-based rigid semiconducting polymers were designed to overcome major limitations in the development of n-type organic thermoelectrics, namely electrical conductivity and air stability. Experimental and theoretical investigations demonstrated that increasing the lactone group density by increasing the benzene content from 0 % benzene (P-0), to 50 % (P-50), and 75 % (P-75) resulted in progressively larger electron affinities (up to 4.37 eV), suggesting a more favorable doping process, when employing (N-DMBI) as the dopant. Larger polaron delocalization was also evident, due to the more planarized conformation, which is proposed to lead to a lower hopping energy barrier. As a consequence, the electrical conductivity increased by three orders of magnitude, to achieve values of up to 12 S cm and Power factors of 13.2 μWm−1 K−2 were thereby enabled. These findings present new insights into material design guidelines for the future development of air stable n-type organic thermoelectrics.

Original languageEnglish (US)
Article numbere202113078
JournalAngewandte Chemie - International Edition
Volume61
Issue number7
DOIs
StatePublished - Feb 7 2022

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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