Surface Functionalization with (3-Glycidyloxypropyl)trimethoxysilane (GOPS) as an Alternative to Blending for Enhancing the Aqueous Stability and Electronic Performance of PEDOT:PSS Thin Films

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Author(s)Osazuwa, Peter O.
Author(s)Lo, Chun-Yuan
Author(s)Feng, Xu
Author(s)Nolin, Abigail
Author(s)Dhong, Charles
Author(s)Kayser, Laure V.
Date Accessioned2024-02-08T17:55:28Z
Date Available2024-02-08T17:55:28Z
Publication Date2023-11-29
DescriptionThis document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Materials and Interfaces, copyright © 2023 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsami.3c09452. This article will be embargoed until 11/29/2024.
AbstractOrganic mixed ionic–electronic conductors, such as poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS), are essential materials for the fabrication of bioelectronic devices due to their unique ability to couple and transport ionic and electronic charges. The growing interest in bioelectronic devices has led to the development of organic electrochemical transistors (OECTs) that can operate in aqueous solutions and transduce ionic signals of biological origin into measurable electronic signals. A common challenge with OECTs is maintaining the stability and performance of the PEDOT:PSS films operating under aqueous conditions. Although the conventional approach of blending the PEDOT:PSS dispersions with a cross-linker such as (3-glycidyloxypropyl)trimethoxysilane (GOPS) helps to ensure strong adhesion of the films to device substrates, it also impacts the morphology and thus electrical properties of the PEDOT:PSS films, which leads to a significant reduction in the performance of OECTs. In this study, we instead functionalize only the surface of the device substrates with GOPS to introduce a silane monolayer before spin-coating the PEDOT:PSS dispersion on the substrate. In all cases, having a GOPS monolayer instead of a blend leads to increased electronic performance metrics, such as three times higher electronic conductivity, volumetric capacitance, and mobility–capacitance product [μC*] value in OECT devices, ultimately leading to a record value of 406 ± 39 F cm–1 V–1 s–1 for amorphous PEDOT:PSS. This increased performance does not come at the expense of operational stability, as both the blend and surface functionalization show similar performance when subjected to pulsed gate bias stress, long-term electrochemical cycling tests, and aging over 150 days. Overall, this study establishes a novel approach to using GOPS as a surface monolayer instead of a blended cross-linker, for achieving high-performance organic mixed ionic–electronic conductors that are stable in water for bioelectronics.
SponsorThe research reported in this publication was supported by a CAREER award from the National Science Foundation (NSF) (grant No. DMR-2237888) and start-up funds from the University of Delaware (UD) to L.V.K. The authors acknowledge the financial support for P.O.O. from the graduate traineeship program NRT-HDR: Computing and Data Science Training for Materials Innovation, Discovery, Analytics (MIDAS) funded by NSF grant No. 2125703. C.D. and A.N. acknowledge support from the NIH-NEI under grant No. R01EY032584-02. The authors thank Dr. Scott Keene for providing the LabVIEW code for the pulsed gate bias stress tests. The authors thank Dr. Lucas Flagg for insightful discussions. The authors thank the Surface Analysis Facility at the University of Delaware for assistance in the XPS, Raman spectroscopy, and ToF-SIMS measurements. The authors thank the DBI Bio-Imaging Center at the University of Delaware for access to the AFM instrument (NIH-NIGMS grant No. P20 GM103446, NSF grant No. IIA-1301765, and the State of Delaware). XPS analysis was performed with the instrument sponsored by the NSF under grant No. CHE-1428149. ToF-SIMS analysis was performed with the instrument sponsored by the NSF under grant No. DMR-2116754.
CitationOsazuwa, Peter O., Chun-Yuan Lo, Xu Feng, Abigail Nolin, Charles Dhong, and Laure V. Kayser. “Surface Functionalization with (3-Glycidyloxypropyl)Trimethoxysilane (GOPS) as an Alternative to Blending for Enhancing the Aqueous Stability and Electronic Performance of PEDOT:PSS Thin Films.” ACS Applied Materials & Interfaces 15, no. 47 (November 29, 2023): 54711–20. https://doi.org/10.1021/acsami.3c09452.
ISSN1944-8252
URLhttps://udspace.udel.edu/handle/19716/33960
Languageen_US
PublisherACS Applied Materials and Interfaces
Keywordsorganic bioelectronics
Keywordswater stability
KeywordsPEDOT:PSS
KeywordsGOPS
Keywordssurface functionalization
Keywordsorganic electrochemical transistor
TitleSurface Functionalization with (3-Glycidyloxypropyl)trimethoxysilane (GOPS) as an Alternative to Blending for Enhancing the Aqueous Stability and Electronic Performance of PEDOT:PSS Thin Films
TypeArticle
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