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Title: High Conductivity and Electron-Transfer Validation in an n-Type Fluoride-Anion-Doped Polymer for Thermoelectrics in Air

Abstract

Air‐stable and soluble tetrabutylammonium fluoride (TBAF) is demonstrated as an efficient n‐type dopant for the conjugated polymer ClBDPPV. Electron transfer from F anions to the π‐electron‐deficient ClBDPPV through anion–π electronic interactions is strongly corroborated by the combined results of electron spin resonance, UV–vis–NIR, and ultraviolet photoelectron spectroscopy. Doping of ClBDPPV with 25 mol% TBAF boosts electrical conductivity to up to 0.62 S cm −1 , among the highest conductivities that have been reported for solution‐processed n‐type conjugated polymers, with a thermoelectric power factor of 0.63 µW m −1 K −2 in air. Importantly, the Seebeck coefficient agrees with recently published correlations to conductivity. Moreover, the F ‐doped ClBDPPV shows significant air stability, maintaining the conductivity of over 0.1 S cm −1 in a thick film after exposure to air for one week, to the best of our knowledge the first report of an air‐stable solution‐processable n‐doped conductive polymer with this level of conductivity. The result shows that using solution‐processable small‐anion salts such as TBAF as an n‐dopant of organic conjugated polymers possessing lower LUMO (lowest unoccupied molecular orbital), less than −4.2 eV) can open new opportunities toward high‐performance air‐stable solution‐processable n‐type thermoelectric (TE) conjugated polymers.

Authors:
 [1];  [2];  [3];  [4];  [1];  [3];  [4];  [5];  [5]; ORCiD logo [6]
  1. Johns Hopkins Univ., Baltimore, MD (United States). Dept. of Materials Science and Engineering
  2. Johns Hopkins Univ., Baltimore, MD (United States). Dept. of Materials Science and Engineering; Univ. of Maryland Baltimore County (UMBC), Baltimore, MD (United States). Dept. of Mechanical Engineering
  3. Johns Hopkins Univ., Baltimore, MD (United States). Dept. of Electrical and Computer Engineering
  4. Johns Hopkins Univ., Baltimore, MD (United States). Dept. of Chemistry
  5. Univ. of Virginia, Charlottesville, VA (United States). Dept. of Mechanical and Aerospace Engineering
  6. Johns Hopkins Univ., Baltimore, MD (United States). Dept. of Materials Science and Engineering. Dept. of Chemistry
Publication Date:
Research Org.:
Johns Hopkins Univ., Baltimore, MD (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Army Research Office (ARO) (United States)
OSTI Identifier:
1533038
Alternate Identifier(s):
OSTI ID: 1380023
Grant/Contract Number:  
FG02-07ER46465; W911NF-16-1-0320
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 29; Journal Issue: 34; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; chemical doping; fluoride salts; n-type conjugated polymers; organic semiconductors; thermoelectrics

Citation Formats

Zhao, Xingang, Madan, Deepa, Cheng, Yan, Zhou, Jiawang, Li, Hui, Thon, Susanna M., Bragg, Arthur E., DeCoster, Mallory E., Hopkins, Patrick E., and Katz, Howard E. High Conductivity and Electron-Transfer Validation in an n-Type Fluoride-Anion-Doped Polymer for Thermoelectrics in Air. United States: N. p., 2017. Web. doi:10.1002/adma.201606928.
Zhao, Xingang, Madan, Deepa, Cheng, Yan, Zhou, Jiawang, Li, Hui, Thon, Susanna M., Bragg, Arthur E., DeCoster, Mallory E., Hopkins, Patrick E., & Katz, Howard E. High Conductivity and Electron-Transfer Validation in an n-Type Fluoride-Anion-Doped Polymer for Thermoelectrics in Air. United States. https://doi.org/10.1002/adma.201606928
Zhao, Xingang, Madan, Deepa, Cheng, Yan, Zhou, Jiawang, Li, Hui, Thon, Susanna M., Bragg, Arthur E., DeCoster, Mallory E., Hopkins, Patrick E., and Katz, Howard E. Fri . "High Conductivity and Electron-Transfer Validation in an n-Type Fluoride-Anion-Doped Polymer for Thermoelectrics in Air". United States. https://doi.org/10.1002/adma.201606928. https://www.osti.gov/servlets/purl/1533038.
@article{osti_1533038,
title = {High Conductivity and Electron-Transfer Validation in an n-Type Fluoride-Anion-Doped Polymer for Thermoelectrics in Air},
author = {Zhao, Xingang and Madan, Deepa and Cheng, Yan and Zhou, Jiawang and Li, Hui and Thon, Susanna M. and Bragg, Arthur E. and DeCoster, Mallory E. and Hopkins, Patrick E. and Katz, Howard E.},
abstractNote = {Air‐stable and soluble tetrabutylammonium fluoride (TBAF) is demonstrated as an efficient n‐type dopant for the conjugated polymer ClBDPPV. Electron transfer from F − anions to the π‐electron‐deficient ClBDPPV through anion–π electronic interactions is strongly corroborated by the combined results of electron spin resonance, UV–vis–NIR, and ultraviolet photoelectron spectroscopy. Doping of ClBDPPV with 25 mol% TBAF boosts electrical conductivity to up to 0.62 S cm −1 , among the highest conductivities that have been reported for solution‐processed n‐type conjugated polymers, with a thermoelectric power factor of 0.63 µW m −1 K −2 in air. Importantly, the Seebeck coefficient agrees with recently published correlations to conductivity. Moreover, the F − ‐doped ClBDPPV shows significant air stability, maintaining the conductivity of over 0.1 S cm −1 in a thick film after exposure to air for one week, to the best of our knowledge the first report of an air‐stable solution‐processable n‐doped conductive polymer with this level of conductivity. The result shows that using solution‐processable small‐anion salts such as TBAF as an n‐dopant of organic conjugated polymers possessing lower LUMO (lowest unoccupied molecular orbital), less than −4.2 eV) can open new opportunities toward high‐performance air‐stable solution‐processable n‐type thermoelectric (TE) conjugated polymers.},
doi = {10.1002/adma.201606928},
journal = {Advanced Materials},
number = 34,
volume = 29,
place = {United States},
year = {Fri Jul 14 00:00:00 EDT 2017},
month = {Fri Jul 14 00:00:00 EDT 2017}
}

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