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Structure and Dopant Engineering in PEDOT Thin Films: Practical Tools for a Dramatic Conductivity Enhancement

Magatte N. Gueye 1, 2 Alexandre Carella 2 Nicolas Massonnet 2 Etienne Yvenou 2 Sophie Brenet 3 Jerome Faure-Vincent 1 Stephanie Pouget 4 Francois Rieutord 5 Hanako Okuno 6 Anass Benayad 2 Renaud Demadrille 1 Jean-Pierre Simonato 2
1 LEMOH - Laboratoire d'Electronique Moléculaire Organique et Hybride
SYMMES - SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé : DRF/INAC/SYMMES
3 CREAB - Chimie pour la Reconnaissance et l’Etude d’Assemblages Biologiques
SYMMES - SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé : DRF/IRIG/SYMMES
4 SGX - Service Général des Rayons X
MEM - Modélisation et Exploration des Matériaux : DRF/IRIG/MEM
5 NRS - Nanostructures et Rayonnement Synchrotron
MEM - Modélisation et Exploration des Matériaux : DRF/IRIG/MEM
6 LEMMA - Laboratoire d'Etude des Matériaux par Microscopie Avancée
MEM - Modélisation et Exploration des Matériaux : DRF/IRIG/MEM
Abstract : Poly(3,4-ethylenedioxythiophene) (PEDOT) is certainly the most known and most used conductive polymer because it is commercially available and shows great potential for organic electronic, photovoltaic, and thermoelectric applications. Studies dedicated to PEDOT films have led to high conductivity enhancements. However, an exhaustive understanding of the mechanisms governing such enhancement is still lacking, hindered by the semicrystalline nature of the material itself. In this article, we report the development of highly conductive PEDOT films by controlling the crystallization of the PEDOT chains and by a subsequent dopant engineering approach using iron(III) trifluoromethanesulfonate as oxidant, N-methyl pyrrolidone as polymerization rate controller and sulfuric as dopant. XRD, HRTEM, Synchrotron GIWAXS analyses and conductivity measurements down to 3 K allowed us to unravel the organization, doping, and transport mechanism of these highly conductive PEDOT materials. N-methyl pyrrolidone promotes bigger crystallites and structure enhancement during polymerization, whereas sulfuric acid treatment allows the replacement of triflate anions by hydrogenosulfate and increases the charge carrier concentration. We finally propose a charge transport model that fully corroborates our experimental observations. These polymers exhibit conductivities up to 5400 S cm(-1) and thus show great promise for room temperature thermoelectric applications or ITO alternative for transparent electrodes.
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Submitted on : Thursday, July 26, 2018 - 3:16:09 PM
Last modification on : Monday, March 29, 2021 - 2:43:03 PM

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Magatte N. Gueye, Alexandre Carella, Nicolas Massonnet, Etienne Yvenou, Sophie Brenet, et al.. Structure and Dopant Engineering in PEDOT Thin Films: Practical Tools for a Dramatic Conductivity Enhancement. Chemistry of Materials, American Chemical Society, 2016, 28 (10), pp.3462-3468. ⟨10.1021/acs.chemmater.6b01035⟩. ⟨cea-01849850⟩

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