eprintid: 10194990 rev_number: 7 eprint_status: archive userid: 699 dir: disk0/10/19/49/90 datestamp: 2024-07-23 16:01:59 lastmod: 2024-07-23 16:01:59 status_changed: 2024-07-23 16:01:59 type: article metadata_visibility: show sword_depositor: 699 creators_name: Gómez, Germán Darío creators_name: Günther, Florian Steffen creators_name: Schroeder, Bob C creators_name: Couto Faria, Gregório title: Synthesis and polymerization of polyelectrolyte-based conductive inks: the protagonism of the coadjutant oxidizing salt ispublished: inpress divisions: UCL divisions: B04 divisions: C06 divisions: F56 note: This version is the author-accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. abstract: Poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) has gained significant popularity as a material in both academic and industrial fields, especially due to the its vast application in electronic-based devices. However, despite its popularity and prominence in organic electronics, there is still a lack of scientific references regarding the synthesis and production of PEDOT:PSS inks. Here, we aim to discuss and elucidate the relationship between the conducting properties of PEDOT:PSS inks and the oxidizing agent concentration used during the oxidative polymerization of EDOT in the presence of PSS. To achieve this, we first studied the effect of addition of an oxidant to PSS solutions via dynamic light scattering (DLS) to characterize whether a higher oxidant concentration impacts the chain conformation of PSS in solution. Furthermore, we conducted UV-Vis spectroscopy measurements at various stages during the synthesis and purification of PEDOT:PSS to assess the formation of polarons and bipolarons. Finally, we evaluated the properties of deposited PEDOT:PSS films. Our findings demonstrate that the addition of an oxidant to PSS solutions leads to polyelectrolyte chain shrinkage, due to the screening of electrostatic interactions between the negatively charged sulfonate groups. Consequently, the likelihood of effective coupling between the PEDOT+ and PSS− counterparts is reduced due to the presence oxidant ions. This hypothesis was confirmed since inks polymerized with a higher oxidant concentration underwent depletion from bipolarons to polarons during the purification process as counterions originating from the oxidizing agent were removed. date: 2024 date_type: published publisher: Royal Society of Chemistry (RSC) official_url: https://doi.org/10.1039/D4PY00574K full_text_type: other language: eng verified: verified_manual elements_id: 2298949 doi: 10.1039/d4py00574k lyricists_name: Schroeder, Bob lyricists_id: BCSCH40 actors_name: Schroeder, Bob actors_id: BCSCH40 actors_role: owner full_text_status: restricted publication: Polymer Chemistry issn: 1759-9954 citation: Gómez, Germán Darío; Günther, Florian Steffen; Schroeder, Bob C; Couto Faria, Gregório; (2024) Synthesis and polymerization of polyelectrolyte-based conductive inks: the protagonism of the coadjutant oxidizing salt. Polymer Chemistry 10.1039/d4py00574k <https://doi.org/10.1039/d4py00574k>. (In press). document_url: https://discovery.ucl.ac.uk/id/eprint/10194990/1/Polymer_chemistry_accepted_manuscript.pdf