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  1. Ion transport in organic mixed ionic-electronic conductors (OMIECs) is crucial due to its direct impact on device response time and operating mechanisms but is often assessed indirectly or necessitates extra assumptions. Operando x-ray fluorescence (XRF) is a powerful, direct probe for elemental characterization of bulk OMIECs and was used to directly quantify ion composition and mobility in a model OMIEC, poly(3,4-ethylenedioxythiophene)-poly(styrene sulfonate) (PEDOT:PSS), during device operation. The first cycle revealed slow electrowetting and cation-proton exchange. Subsequent cycles showed rapid response with minor cation fluctuation (~5%). Comparison with optical-tracked electrochromic fronts revealed mesoscale structure–dependent proton transport. The calculated effective ion mobility demonstrated thickness-dependent behavior, emphasizing an interfacial ion transport pathway with a higher mobile ion density. The decoupling of interfacial effects on bulk ion mobility and the decoupling of cation and proton migration elucidate ion transport in conventional and emerging OMIEC-based devices and has broader implications for other ionic conductors writ large. 
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    Free, publicly-accessible full text available April 26, 2025
  2. Abstract

    Developing nerve grafts with intact mesostructures, superior conductivity, minimal immunogenicity, and improved tissue integration is essential for the treatment and restoration of neurological dysfunctions. A key factor is promoting directed axon growth into the grafts. To achieve this, biohybrid nerves are developed using decellularized rat sciatic nerve modified by in situ polymerization of poly(3,4‐ethylenedioxythiophene) (PEDOT). Nine biohybrid nerves are compared with varying polymerization conditions and cycles, selecting the best candidate through material characterization. These results show that a 1:1 ratio of FeCl3oxidant to ethylenedioxythiophene (EDOT) monomer, cycled twice, provides superior conductivity (>0.2 mS cm−1), mechanical alignment, intact mesostructures, and high compatibility with cells and blood. To test the biohybrid nerve's effectiveness in promoting motor axon growth, human Spinal Cord Spheroids (hSCSs) derived from HUES 3 Hb9:GFP cells are used, with motor axons labeled with green fluorescent protein (GFP). Seeding hSCS onto one end of the conduit allows motor axon outgrowth into the biohybrid nerve. The construct effectively promotes directed motor axon growth, which improves significantly after seeding the grafts with Schwann cells. This study presents a promising approach for reconstructing axonal tracts in humans.

     
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  3. Abstract Organic electrochemical transistors are a promising technology for bioelectronic devices, with applications in neuromorphic computing and healthcare. The active component enabling an organic electrochemical transistor is the organic mixed ionic-electronic conductor whose optimization is critical for realizing high-performing devices. In this study, the influence of purity and molecular weight is examined for a p-type polythiophene and an n-type naphthalene diimide-based polymer in improving the performance and safety of organic electrochemical transistors. Our preparative GPC purification reduced the Pd content in the polymers and improved their organic electrochemical transistor mobility by ~60% and 80% for the p- and n-type materials, respectively. These findings demonstrate the paramount importance of removing residual Pd, which was concluded to be more critical than optimization of a polymer’s molecular weight, to improve organic electrochemical transistor performance and that there is readily available improvement in performance and stability of many of the reported organic mixed ionic-electronic conductors. 
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  4. Organic electrochemical transistors (OECTs) are highly versatile in terms of their form factor, fabrication approach that can be applied, and freedom in the choice of substrate material. Their ability to transduce ionic into electric signals and the use of bio-compatible organic materials makes them ideally suited for a wide range of applications, in particular in areas where electronic circuits are interfaced with biologic matter. OECT technology has attracted widespread interest in recent years, which has been accompanied by a steady increase in its performance. However, this progress was mainly driven by device optimization and less by targeting the design of new device geometries and OECT materials. To narrow this gap, this review provides an overview on the different device models that are used to explain the underlying physics governing the steady and transient behavior of OECTs. We show how the models can be used to identify synthetic targets to produce higher performing OECT materials and summarize recently reported materials classes. Overall, a road-map of future research in new device models and material design is presented summarizing the most pressing open questions in the understanding of OECTs. 
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  5. Electrical stimulation has shown promise in clinical studies to treat nerve injuries. This work is aimed to create an aligned bioelectronic construct that can be used to bridge a nerve gap, directly interfacing with the damaged nerve tissue to provide growth support. The conductive three‐dimensional bioelectronic scaffolds described herein are composite materials, comprised of conductive polypyrrole (PPy) nanoparticles embedded in an aligned collagen hydrogel. The bioelectronic constructs are seeded with dorsal root ganglion derived primary rat neurons and electrically stimulated in vitro. The PPy loaded constructs support a 1.7‐fold increase in neurite length in comparison to control collagen constructs. Furthermore, upon electrical stimulation of the PPy‐collagen construct, a 1.8‐fold increase in neurite length is shown. This work illustrates the potential of bioelectronic constructs in neural tissue engineering and lays the groundwork for the development of novel bioelectronic materials for neural interfacing applications.

     
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  6. Abstract

    Conductive polymers (CPs) are widely studied for their ability to influence a myriad of tissue systems. While their mixed ionic/electronic conductivity is commonly considered the primary driver of these benefits, the mechanisms by which CPs influence cell fate remain unclear. In this study, CP‐biomaterial interactions are investigated using collagen, due to its widespread prevalence throughout the body and in tissue engineering constructs. Collagen is functionalized with both electrostatically and covalently bound derivatives of the CP poly(3,4‐ethylenedioxythiophene) (PEDOT) doped via backbone‐tethered sulfonate groups, which enable high solubility and loading to the collagen biomatrix. Intrinsically doped scaffolds are compared to those incorporated with a commercially available PEDOT formulation, which is complexed with polyanionic polystyrene sulfonate (PSS). Low loadings of intrinsically doped PEDOT do not increase substrate conductivity compared to collagen alone, enabling separate investigation into CP loading and conductivity. Interestingly, higher PEDOT loading bolsters human mesenchymal stromal (hMSC) cell gene expression of Oct‐4 and NANOG, which are key transcription factors regulating cell stemness. Conductive collagen composites with commercial PEDOT:PSS do not significantly affect the expression of these transcription factors in hMSCs. Furthermore, it is demonstrated that PEDOT regulates cellular fate independently from physical changes to the material but directly to the loading of the polymer.

     
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