Intrinsically Stretchable Block Copolymer Based on PEDOT:PSS for Improved Performance in Bioelectronic Applications

The conductive polyelectrolyte complex poly­(3,4-ethylenedioxythiophene):poly­(styrenesulfonate) (PEDOT:PSS) is ubiquitous in research dealing with organic electronic devices (e.g., solar cells, wearable and implantable sensors, and electrochemical transistors). In many bioelectronic applications, t...

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Bibliographic Details
Published in:ACS applied materials & interfaces 2022-02, Vol.14 (4), p.4823-4835
Main Authors: Blau, Rachel, Chen, Alexander X, Polat, Beril, Becerra, Laura L, Runser, Rory, Zamanimeymian, Beeta, Choudhary, Kartik, Lipomi, Darren J
Format: Article
Language:English
Subjects:
Biocompatible Materials - chemistry
Biological and Medical Applications of Materials and Interfaces
Biosensing Techniques
Bridged Bicyclo Compounds, Heterocyclic - chemistry
Electric Conductivity
Materials Testing
Particle Size
Polymers - chemistry
Polystyrenes - chemistry
Surface Properties
Tensile Strength
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Summary:The conductive polyelectrolyte complex poly­(3,4-ethylenedioxythiophene):poly­(styrenesulfonate) (PEDOT:PSS) is ubiquitous in research dealing with organic electronic devices (e.g., solar cells, wearable and implantable sensors, and electrochemical transistors). In many bioelectronic applications, the applicability of commercially available formulations of PEDOT:PSS (e.g., Clevios) is limited by its poor mechanical properties. Additives can be used to increase the compliance but pose a risk of leaching, which can result in device failure and increased toxicity (in biological settings). Thus, to increase the mechanical compliance of PEDOT:PSS without additives, we synthesized a library of intrinsically stretchable block copolymers. In particular, controlled radical polymerization using a reversible addition–fragmentation transfer process was used to generate block copolymers consisting of a block of PSS (of fixed length) appended to varying blocks of poly­(poly­(ethylene glycol) methyl ether acrylate) (PPEGMEA). These block copolymers (PSS(1)-b-PPEGMEA(x), where x ranges from 1 to 6) were used as scaffolds for oxidative polymerization of PEDOT. By increasing the lengths of the PPEGMEA segments on the PEDOT:[PSS(1)-b-PPEGMEA(1–6)] block copolymers, (“Block-1” to “Block-6”), or by blending these copolymers with PEDOT:PSS, the mechanical and electronic properties of the polymer can be tuned. Our results indicate that the polymer with the longest block of PPEGMEA, Block-6, had the highest fracture strain (75%) and lowest elastic modulus (9.7 MPa), though at the expense of conductivity (0.01 S cm–1). However, blending Block-6 with PEDOT:PSS to compensate for the insulating nature of the PPEGMEA resulted in increased conductivity [2.14 S cm–1 for Blend-6 (2:1)]. Finally, we showed that Block-6 outperforms a commercial formulation of PEDOT:PSS as a dry electrode for surface electromyography due to its favorable mechanical properties and better adhesion to skin.
ISSN:1944-8244
1944-8252
DOI:10.1021/acsami.1c18495