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

Maryam Alsufyani, Marc-Antoine Stoeckel, Xingxing Chen, Karl Thorely, 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

Research output: Contribution to journalArticlepeer-review

29 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)
JournalAngewandte Chemie International Edition
DOIs
StatePublished - Nov 19 2021

Bibliographical note

KAUST Repository Item: Exported on 2021-11-24
Acknowledged KAUST grant number(s): OSR-2018-CRG/CCF-3079, OSR-2018-CRG7-3749, OSR-2019-CRG8-4086
Acknowledgements: We acknowledge financial support from KAUST, including Office of Sponsored Research (OSR) awards no. OSR-2018-CRG/CCF-3079, OSR-2019-CRG8-4086 and OSR-2018-CRG7-3749. We acknowledge funding from ERC Synergy Grant SC2 (610115), the european union horizon 2020 research and innovation programme under grant agreement n°952911, project BOOSTER and grant agreement n°862474, project RoLA-FLEX, as well as EPSRC Project EP/T026219/1B.D.P. and J.R. gratefully acknowledge support from the National Science Foundation grant no. NSF DMR-1751308. This research used resources of the Advanced Photon Source (beamline 8-ID-E), a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. The work at Linköping University was financially supported by the Knut and Alice Wallenberg foundation, the Swedish Research Council (2020 03243), Olle Engkvists Stiftelse (204-0256), the EC for the ITN projects HORATES (GA-955837), and the Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linköping University (Faculty Grant SFO-Mat-LiU 2009-00971).

ASJC Scopus subject areas

  • General Chemistry
  • Catalysis

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