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Method Matters : Exploring Alkoxysulfonate-Functionalized Poly(3,4-ethylenedioxythiophene) and Its Unintentional Self-Aggregating Copolymer toward Injectable Bioelectronics

Mousa, Abdelrazek H. LU ; Bliman, David LU ; Hiram Betancourt, Lazaro LU ; Hellman, Karin LU ; Ekström, Peter LU ; Savvakis, Marios ; Strakosas, Xenofon LU ; Marko-Varga, György LU ; Berggren, Magnus and Hjort, Martin LU orcid , et al. (2022) In Chemistry of Materials 34(6). p.2752-2763
Abstract

Injectable bioelectronics could become an alternative or a complement to traditional drug treatments. To this end, a new self-doped p-type conducting PEDOT-S copolymer (A5) was synthesized. This copolymer formed highly water-dispersed nanoparticles and aggregated into a mixed ion-electron conducting hydrogel when injected into a tissue model. First, we synthetically repeated most of the published methods for PEDOT-S at the lab scale. Surprisingly, analysis using high-resolution matrix-assisted laser desorption ionization-mass spectroscopy showed that almost all the methods generated PEDOT-S derivatives with the same polymer lengths (i.e., oligomers, seven to eight monomers in average); thus, the polymer length cannot account for the... (More)

Injectable bioelectronics could become an alternative or a complement to traditional drug treatments. To this end, a new self-doped p-type conducting PEDOT-S copolymer (A5) was synthesized. This copolymer formed highly water-dispersed nanoparticles and aggregated into a mixed ion-electron conducting hydrogel when injected into a tissue model. First, we synthetically repeated most of the published methods for PEDOT-S at the lab scale. Surprisingly, analysis using high-resolution matrix-assisted laser desorption ionization-mass spectroscopy showed that almost all the methods generated PEDOT-S derivatives with the same polymer lengths (i.e., oligomers, seven to eight monomers in average); thus, the polymer length cannot account for the differences in the conductivities reported earlier. The main difference, however, was that some methods generated an unintentional copolymer P(EDOT-S/EDOT-OH) that is more prone to aggregate and display higher conductivities in general than the PEDOT-S homopolymer. Based on this, we synthesized the PEDOT-S derivative A5, that displayed the highest film conductivity (33 S cm-1) among all PEDOT-S derivatives synthesized. Injecting A5 nanoparticles into the agarose gel cast with a physiological buffer generated a stable and highly conductive hydrogel (1-5 S cm-1), where no conductive structures were seen in agarose with the other PEDOT-S derivatives. Furthermore, the ion-treated A5 hydrogel remained stable and maintained initial conductivities for 7 months (the longest period tested) in pure water, and A5 mixed with Fe3O4 nanoparticles generated a magnetoconductive relay device in water. Thus, we have successfully synthesized a water-processable, syringe-injectable, and self-doped PEDOT-S polymer capable of forming a conductive hydrogel in tissue mimics, thereby paving a way for future applications within in vivo electronics.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Chemistry of Materials
volume
34
issue
6
pages
2752 - 2763
publisher
The American Chemical Society (ACS)
external identifiers
  • pmid:35360437
  • scopus:85126111159
ISSN
0897-4756
DOI
10.1021/acs.chemmater.1c04342
language
English
LU publication?
yes
additional info
Funding Information: This study was accomplished within MultiPark, NanoLund and Materials Science on Advanced Functional Materials─Strategic Research Areas at Lund University and Linköping University, respectively. This work was supported by Swedish Research Council (2018-05258 and 2018-06197), Swedish Foundation for Strategic Research (e-NeuroPharmacology, RMX18-0083), and the European Research Council (ERC) project (e-NeuroPharma 834677). The cation exchange resin was provided by Lanxess AG. Publisher Copyright: © 2022 The Authors. Published by American Chemical Society.
id
dc39e2e7-8208-4316-8f95-81c53505544e
date added to LUP
2022-03-20 20:51:38
date last changed
2024-06-19 05:12:05
@article{dc39e2e7-8208-4316-8f95-81c53505544e,
  abstract     = {{<p>Injectable bioelectronics could become an alternative or a complement to traditional drug treatments. To this end, a new self-doped p-type conducting PEDOT-S copolymer (A5) was synthesized. This copolymer formed highly water-dispersed nanoparticles and aggregated into a mixed ion-electron conducting hydrogel when injected into a tissue model. First, we synthetically repeated most of the published methods for PEDOT-S at the lab scale. Surprisingly, analysis using high-resolution matrix-assisted laser desorption ionization-mass spectroscopy showed that almost all the methods generated PEDOT-S derivatives with the same polymer lengths (i.e., oligomers, seven to eight monomers in average); thus, the polymer length cannot account for the differences in the conductivities reported earlier. The main difference, however, was that some methods generated an unintentional copolymer P(EDOT-S/EDOT-OH) that is more prone to aggregate and display higher conductivities in general than the PEDOT-S homopolymer. Based on this, we synthesized the PEDOT-S derivative A5, that displayed the highest film conductivity (33 S cm-1) among all PEDOT-S derivatives synthesized. Injecting A5 nanoparticles into the agarose gel cast with a physiological buffer generated a stable and highly conductive hydrogel (1-5 S cm-1), where no conductive structures were seen in agarose with the other PEDOT-S derivatives. Furthermore, the ion-treated A5 hydrogel remained stable and maintained initial conductivities for 7 months (the longest period tested) in pure water, and A5 mixed with Fe3O4 nanoparticles generated a magnetoconductive relay device in water. Thus, we have successfully synthesized a water-processable, syringe-injectable, and self-doped PEDOT-S polymer capable of forming a conductive hydrogel in tissue mimics, thereby paving a way for future applications within in vivo electronics. </p>}},
  author       = {{Mousa, Abdelrazek H. and Bliman, David and Hiram Betancourt, Lazaro and Hellman, Karin and Ekström, Peter and Savvakis, Marios and Strakosas, Xenofon and Marko-Varga, György and Berggren, Magnus and Hjort, Martin and Ek, Fredrik and Olsson, Roger}},
  issn         = {{0897-4756}},
  language     = {{eng}},
  number       = {{6}},
  pages        = {{2752--2763}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{Chemistry of Materials}},
  title        = {{Method Matters : Exploring Alkoxysulfonate-Functionalized Poly(3,4-ethylenedioxythiophene) and Its Unintentional Self-Aggregating Copolymer toward Injectable Bioelectronics}},
  url          = {{http://dx.doi.org/10.1021/acs.chemmater.1c04342}},
  doi          = {{10.1021/acs.chemmater.1c04342}},
  volume       = {{34}},
  year         = {{2022}},
}