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The low sensitivity of liquid-state nuclear magnetic resonance (NMR) can be overcome by hyperpolarizing nuclear spins by dissolution dynamic nuclear polarization (dDNP). It consists of transferring the near-unity polarization of unpaired electron spins of stable radicals to the nuclear spins of interest at liquid helium temperatures, below 2 K, before melting the sample in view of hyperpolarized liquid-state magnetic resonance experiments. Reaching such a temperature is challenging and requires complex instrumentation, which impedes the deployment of dDNP. Here, we propose organic conductive polymers such as polyaniline (PANI) as a new class of polarizing matrices and report 1H polarizations of up to 5%. We also show that 13C spins of a host solution impregnated in porous conductive polymers can be hyperpolarized by relayed DNP. Such conductive polymers can be synthesized as chiral and display current induced spin selectivity leading to electron spins hyperpolarization close to unity without the need for low temperatures nor high magnetic fields. Our results show the feasibility of solid-state DNP in conductive polymers that are known to exhibit chirality-induced spin selectivity.

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The development of alternative conductive polymers for the well-known poly (3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) is of great significance for improving the stability in long-term using and high-temperature environments. Herein, an innovative PEDOT:S-ANF aqueous dispersion is successfully prepared by using sulfamic acid (SA) to modified aramid nanofibers (S-ANF) as an alternative dispersant for PSS and the subsequent in situ polymerization of PEDOT. Thanks to the excellent film forming ability and surface negative groups of S-ANF, the PEDOT:S-ANF films show comparable tensile strength and elongation to unmodified PEDOT:ANF. Meanwhile, PEDOT:S-ANF has a high conductivity of 27.87 S cm-1, which is more than 20 times higher than that of PEDOT:PSS. The film exhibits excellent electromagnetic interference (EMI) shielding and thermoelectric performance, with a shielding effectiveness (SE) of 31.14 dB and a power factor (PF) of 0.43 µW m-1K-2. As a substitute for PSS, S-ANF exhibits significant structural and physicochemical properties, resulting in excellent chemical and thermal stability. Even under harsh conditions such as immersing to 0.1 M HCl, 0.1 M NaOH, and 3.5% NaCl solution, or high temperature conditions, the PEDOT:S-ANF films still maintain exceptional EMI shielding performance. Therefore, this multifunctional conductive polymer exhibits enormous potential and even proves its reliability in extreme situations.

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n-Type polythiophene represents a promising category of n-type polymer thermoelectric materials known for their straightforward structure and scalable synthesis. However, n-type polythiophene often suffers from a twisted backbone and poor stacking property when introducing high-density electron-withdrawing groups for a lower lowest unoccupied molecular orbital (LUMO) level, which is considered to be beneficial for n-doping efficiency. Herein, we developed two isomers of polythiophene derivatives, PTTz1 and PTTz2, by inserting thiazole units into the polythiophene backbone composed of thieno[3,4-c]pyrrole-4,6-dione (TPD) and thiophene-3,4-dicarbonitrile (2CNT). Although PTTz1 and PTTz2 share a similar polymer skeleton, they differ in thiazole configuration, with the nitrogen atoms of the thiazole units oriented toward TPD and 2CNT, respectively. The insertion of thiazole units significantly planarizes the polythiophene backbone while largely preserving low LUMO levels. Notably, PTTz2 exhibits a more coplanar backbone and closer π-stacking compared to PTTz1, resulting in a greatly enhanced electron mobility. Both PTTz1 and PTTz2 can be easily n-doped due to their deep LUMO levels. PTTz2 demonstrates superior thermoelectric performance, with an electrical conductivity of 50.3 S cm-1 and a power factor of 23.8 µW m-1 K-2, which is approximately double that of PTTz1. This study highlights the impact of the thiazole unit on n-type polythiophene derivatives and provides valuable guidelines for the design of high-performance n-type polymer thermoelectric materials.

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The diagnosis of diabetes mellitus (DM) affecting 537 million adults worldwide relies on invasive and costly enzymatic methods that have limited stability. Electroactive polypyrrole (PPy)-based molecularly imprinted polymer nanoparticles (eMIPs) have been developed that rival the affinity of enzymes whilst being low-cost, highly robust, and facile to produce. By drop-casting eMIPs onto low-cost disposable screen-printed electrodes (SPEs), sensors have been manufactured that can electrochemically detect glucose in a wide dynamic range (1 µm-10 mm) with a limit of detection (LOD) of 26 nm. The eMIPs sensors exhibit no cross reactivity to similar compounds and negligible glucose binding to non-imprinted polymeric nanoparticles (eNIPs). Measurements of serum samples of diabetic patients demonstrate excellent correlation (>0.93) between these eMIPs sensor and the current gold standard Roche blood analyzer test. Finally, the eMIPs sensors are highly durable and reproducible (storage >12 months), showcasing excellent robustness and thermal and chemical stability. Proof-of-application is provided via measuring glucose using these eMIPs sensor in a two-electrode configuration in spiked artificial interstitial fluid (AISF), highlighting its potential for non-invasive wearable monitoring. Due to the versatility of the eMIPs that can be adapted to virtually any target, this platform technology holds high promise for sustainable healthcare applications via providing rapid detection, low-cost, and inherent robustness.

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Three-dimensional (3D) scaffolds provide cell support while improving tissue regeneration through amplified cellular responses between implanted materials and native tissues. So far, highly conductive cardiac, nerve, and muscle tissues have been engineered by culturing stem cells on electrically inert scaffolds. These scaffolds, even though suitable, may not be very useful compared to the results shown by cells when cultured on conductive scaffolds. Noticing the mature phenotype the stem cells develop over time when cultured on conductive scaffolds, scientists have been trying to impart conductivity to traditionally nonconductive scaffolds. One way to achieve this goal is to blend conductive polymers (polyaniline, polypyrrole, PEDOT:PSS) with inert biomaterials and produce a 3D scaffold using various fabrication techniques. One such technique is projection micro-stereolithography, which is an additive manufacturing technique. It uses a photosensitive solution blended with conductive polymers and uses visible/UV light to crosslink the solution. 3D scaffolds with complex architectural features down to microscale resolution can be printed with this technique promptly. This chapter reports a protocol to fabricate electrically conductive scaffolds using projection micro-stereolithography.

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Porous conductive polymer structures, in particular Poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) structures, are gaining in importance due to their versatile fields of application as sensors, hydrogels, or supercapacitors, to name just a few. Moreover, (porous) conducting polymers have become of interest for wearable and smart textile applications due to their biocompatibility, which enables applications with direct skin contact. Therefore, there is a huge need to investigate distinct, straightforward, and textile-compatible production methods for the fabrication of porous PEDOT:PSS structures. Here, we present novel and uncomplicated approaches to producing diverse porous PEDOT:PSS structures and characterize them thoroughly in terms of porosity, electrical resistance, and their overall appearance. Production methods comprise the incorporation of micro cellulose, the usage of a blowing agent, creating a sponge-like structure, and spraying onto a porous base substrate. This results in the fabrication of various porous structures, ranging from thin and slightly porous to thick and highly porous. Depending on the application, these structures can be modified and integrated into electronic components or wearables to serve as porous electrodes, sensors, or other functional devices.

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Transition metal coordination polymers (TM-CP) are promising inexpensive and flexible electrocatalysts for oxygen evolution reaction in water electrolysis, while their facile synthesis and controllable regulation remain challenging. Here we report an anodic oxidation-electrodeposition strategy for the growth of TM-CP (TM=Fe, Co, Ni, Cr, Mn; CP=polyaniline, polypyrrole) films on a variety of metal substrates that act as both catalyst supports and metal ion sources. An exemplified bimetallic NiFe-polypyrrole (NiFe-PPy) features superior mechanical stability in friction and exhibits high activity with long-term durability in alkaline seawater (over 2000 h) and anion exchange membrane electrolyzer devices at current density of 500 mA cm-2. Spectroscopic and microscopic analysis unravels the configurations with atomically distributed metal sites induced by d-π conjugation, which transforms into a mosaic structure with NiFe (oxy)hydroxides embedded in PPy matrix during oxygen evolution. The superior catalytic performance is ascribed to the anchoring effect of PPy that inhibits metal dissolution, the strong substrate-to-catalyst interaction that ensures good adhesion, and the Fe/Ni-N coordination that modulates the electronic structures to facilitate the deprotonation of *OOH intermediate. This work provides a general strategy and mechanistic insight into building robust inorganic/polymer composite electrodes for oxygen electrocatalysis.

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Electrochemical sensors play a pivotal role in various fields, such as biomedicine and environmental detection, due to their exceptional sensitivity, selectivity, stability, rapid response time, user-friendly operation, and ease of miniaturization and integration. In addition to the research conducted in the application field, significant focus is placed on the selection and optimization of electrode interface materials for electrochemical sensors. The detection performance of these sensors can be significantly enhanced by modifying the interface of either inorganic metal electrodes or printed electrodes. Among numerous available modification materials, conductive polymers (CPs) possess not only excellent conductivity exhibited by inorganic conductors but also unique three-dimensional structural characteristics inherent to polymers. This distinctive combination allows CPs to increase active sites during the detection process while providing channels for rapid ion transmission and facilitating efficient electron transfer during reaction processes. This review article primarily highlights recent research progress concerning CPs as an ideal choice for modifying electrochemical sensors owing to their remarkable features that make them well-suited for biomedical and environmental applications.

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The advent of closed-loop bionics has created a demand for electrode materials that are ideal for both stimulating and recording applications. The growing complexity and diminishing size of implantable devices for neural interfaces have moved beyond what can be achieved with conventional metallic electrode materials. Polymeric electrode materials are a recent development based on polymer composites of organic conductors such as conductive polymers. These materials present exciting new opportunities in the design and fabrication of next-generation electrode arrays which can overcome the electrochemical and mechanical limitations of conventional electrode materials. This review will examine the recent developments in polymeric electrode materials, their application as stimulating and recording electrodes in bionic devices, and their impact on the development of soft, conformal, and high-density neural interfaces.

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The field of biomimetic electronics that mimic synaptic functions has expanded significantly to overcome the limitations of the von Neumann bottleneck. However, the scaling down of the technology has led to an increasingly intricate manufacturing process. To address the issue, this work presents a one-shot integrable electropolymerization (OSIEP) method with remote controllability for the deposition of synaptic elements on a chip by exploiting bipolar electrochemistry. Condensing synthesis, deposition, and patterning into a single fabrication step is achieved by combining alternating-current voltage superimposed on direct-current voltage-bipolar electropolymerization and a specially designed dual source/drain bipolar electrodes. As a result, uniform 6 × 5 arrays of poly(3,4-ethylenedioxythiophene) channels are successfully fabricated on flexible ultrathin parylene substrates in one-shot process. The channels exhibited highly uniform characteristics and are directly used as electrochemical synaptic transistor with synaptic plasticity over 100 s. The synaptic transistors have demonstrated promising performance in an artificial neural network (NN) simulation, achieving a high recognition accuracy of 95.20%. Additionally, the array of synaptic transistor is easily reconfigured to a multi-gate synaptic circuit to implement the principles of operant conditioning. These results provide a compelling fabrication strategy for realizing cost-effective and disposable NN systems with high integration density.

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In the context of improving aircraft safety, this work focuses on creating and testing a graphene-based ice detection system in an environmental chamber. This research is driven by the need for more accurate and efficient ice detection methods, which are crucial in mitigating in-flight icing hazards. The methodology employed involves testing flat graphene-based sensors in a controlled environment, simulating a variety of climatic conditions that could be experienced in an aircraft during its entire flight. The environmental chamber enabled precise manipulation of temperature and humidity levels, thereby providing a realistic and comprehensive test bed for sensor performance evaluation. The results were significant, revealing the graphene sensors' heightened sensitivity and rapid response to the subtle changes in environmental conditions, especially the critical phase transition from water to ice. This sensitivity is the key to detecting ice formation at its onset, a critical requirement for aviation safety. The study concludes that graphene-based sensors tested under varied and controlled atmospheric conditions exhibit a remarkable potential to enhance ice detection systems for aircraft. Their lightweight, efficient, and highly responsive nature makes them a superior alternative to traditional ice detection technologies, paving the way for more advanced and reliable aircraft safety solutions.

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Controlled release systems have gained considerable attention owing to their potential to deliver molecules, including ions and drugs, in a customized manner. We present a light-induced ion-transfer platform consisting of a dispersion of nanoparticles (NPs, ~300 nm) with the conductive polymer poly(3-octylthiophene-2,5-diyl) (POT) in the core and a potassium (K+)-selective membrane in the shell. Owing to the photoactive nature of POT, POT NPs can be used for a dual purpose: as a host for positively charged species and as an actuator to trigger the subsequent release. POT0 and doped POT+ coexist in the core, allowing K+ encapsulation in the shell. As POT0 is photo-oxidized to POT+, K+ is released to the (aqueous) dispersion phase to preserve the neutrality of the NPs. This process is reversible and can be simultaneously assessed using the native fluorescence of POT0 and via potentiometric measurements. The NP structure and its mechanism of action were thoroughly studied with a series of control experiments and complementary techniques. Understanding the NP and its surrounding interactions will pave the way for other nanostructured systems, facilitating sophisticated applications. The delivery of ionic drugs and interference/pollutant catching for advanced sensing/restoration will be considered in future research.

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Organic electrochemical transistors (OECTs) employing conductive polymers (CPs) have gained remarkable prominence and have undergone extensive advancements in wearable and implantable bioelectronic applications in recent years. Among the diverse arrays of CPs, poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) is a common choice for the active-layer channel in p-type OECTs, showing a remarkably high transconductance for the high amplification of signals in biosensing applications. This investigation focuses on the novel engineering of PEDOT:PSS composite materials by seamlessly integrating several additives, namely, dimethyl sulfoxide (DMSO), (3-glycidyloxypropyl)trimethoxysilane (GOPS), and a nonionic fluorosurfactant (NIFS), to fine-tune their electrical conductivity, self-healing capability, and stretchability. To elucidate the intricate influences of the DMSO, GOPS, and NIFS additives on the formation of PEDOT:PSS composite films, theoretical calculations were performed, encompassing the solubility parameters and surface energies of the constituent components of the NIFS, PEDOT, PSS, and PSS-GOPS polymers. Furthermore, we conducted a comprehensive array of material analyses, which reveal the intricacies of the phase separation phenomenon and its interaction with the materials' characteristics. Our research identified the optimal composition for the PEDOT:PSS composite films, characterized by outstanding self-healing and stretchable capabilities. This composition has proven to be highly effective for constructing an active-layer channel in the form of OECT-based biosensors fabricated onto polydimethylsiloxane substrates for detecting dopamine. Overall, these findings represent significant progress in the application of PEDOT:PSS composite films in wearable bioelectronics and pave the way for the development of state-of-the-art biosensing technologies.

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This study aims to develop a microelectrode array-based neural probe that can record dopamine activity with high stability and sensitivity. To mimic the high stability of the gold standard method (carbon fiber electrodes), the microfabricated platinum microelectrode is coated with carbon-based nanomaterials. Carboxyl-functionalized multi-walled carbon nanotubes (COOH-MWCNTs) and carbon quantum dots (CQDs) were selected for this purpose, while a conductive polymer like poly (3-4-ethylene dioxythiophene) (PEDOT) or polypyrrole (PPy) serves as a stable interface between the platinum of the electrode and the carbon-based nanomaterials through a co-electrodeposition process. Based on our comparison between different conducting polymers and the addition of CQD, the CNT-CQD-PPy modified microelectrode outperforms its counterparts: CNT-CQD-PEDOT, CNT-PPy, CNT-PEDOT, and bare Pt microelectrode. The CNT-CQD-PPy modified microelectrode has a higher conductivity, stability, and sensitivity while achieving a remarkable limit of detection (LOD) of 35.20 ± 0.77 nM. Using fast-scan cyclic voltammetry (FSCV), these modified electrodes successfully measured dopamine's redox peaks while exhibiting consistent and reliable responses over extensive use. This electrode modification not only paves the way for real-time, precise dopamine sensing using microfabricated electrodes but also offers a novel electrochemical sensor for in vivo studies of neural network dynamics and neurological disorders.

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Chiral two-dimensional (2D) conductive polymers, encompassing chiral, 2D, flexible, and conductive properties, constitute a novel class of material that remains largely unexplored. The infusion of chirality into 2D conductive polymers taps into the unique characteristics associated with chirality, presenting opportunities to enhance or tailor the electronic, optical, and structural properties of materials for specific technological applications. In this study, we synthesized a chiral 2D PEDOT:PMo11V nanofilm through interfacial polymerization, effectively integrating a chiral monolayer, conductive polymer, and inorganic cluster. The inclusion of inorganic cluster serves to enhance the conductivity of the resulting chiral nanofilm. Furthermore, we demonstrated the chiral nanofilm as a capable electrochemical sensor for detecting drug enantiomers. The inherent flexibility of the chiral nanofilm also lays the groundwork for the development of chiral flexible/wearable devices.

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The study has developed two hemi-isoindigo (HID)-based polymers for printed flexible resistor-type nitrogen oxide (NO2 ) sensors: poly[2-ethylhexyl 3-((3'",4'-bis(dodecyloxy)-3,4-dimethoxy-[2,2':5',2'"-terthiophen]-5-yl)methylene)-2-oxoindoline-1-carboxylate] (P1) and poly[2-ethylhexyl 2-oxo-3-((3,3'",4,4'-tetrakis(dodecyloxy)-[2,2':5',2'"-terthiophen]-5-yl)methylene)indoline-1-carboxylate] (P2). These polymers feature thermally removable carbamate side chains on the HID units, providing solubility and creating molecular cavities after thermal annealing. These cavities enhance NO2 diffusion, and the liberated unsubstituted amide ─C(═O)NH─ groups readily form robust double hydrogen bonds (DHB), as demonstrated by computer simulations. Furthermore, both polymers possess elevated highest occupied molecular orbital (HOMO) energy levels of -4.74 and -4.77 eV, making them highly susceptible to p-doping by NO2 . Gas sensors fabricated from P1 and P2 films, anneal under optimized conditions to partially remove carbamate side chains, exhibit remarkable sensitivities of +1400% ppm-1 and +3844% ppm-1 , and low detection limit (LOD) values of 514 ppb and 38.9 ppb toward NO2 , respectively. These sensors also demonstrate excellent selectivity for NO2 over other gases.

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Objective. The controlled delivery of potassium is an interesting neuromodulation modality, being potassium ions involved in shaping neuron excitability, synaptic transmission, network synchronization, and playing a key role in pathological conditions like epilepsy and spreading depression. Despite many successful examples of pre-clinical devices able to influence the extracellular potassium concentration, computational frameworks capturing the corresponding impact on neuronal activity are still missing.Approach. We present a finite-element model describing a PEDOT:PSS-coated microelectrode (herein, simplyionic actuator) able to release potassium and thus modulate the activity of a cortical neuron in anin-vitro-like setting. The dynamics of ions in the ionic actuator, the neural membrane, and the cellular fluids are solved self-consistently.Main results. We showcase the capability of the model to describe on a physical basis the modulation of the intrinsic excitability of the cell and of the synaptic transmission following the electro-ionic stimulation produced by the actuator. We consider three case studies for the ionic actuator with different levels of selectivity to potassium: ideal selectivity, no selectivity, and selectivity achieved by embedding ionophores in the polymer.Significance. This work is the first step toward a comprehensive computational framework aimed to investigate novel neuromodulation devices targeting specific ionic species, as well as to optimize their design and performance, in terms of the induced modulation of neural activity.

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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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Cardiovascular diseases are a leading cause of mortality and pose a significant burden on healthcare systems worldwide. Despite remarkable progress in medical research, the development of effective cardiovascular drugs has been hindered by high failure rates and escalating costs. One contributing factor is the limited availability of mature cardiomyocytes (CMs) for accurate disease modeling and drug screening. Human induced pluripotent stem cell-derived CMs offer a promising source of CMs; however, their immature phenotype presents challenges in translational applications. This review focuses on the road to achieving mature CMs by summarizing the major differences between immature and mature CMs, discussing the importance of adult-like CMs for drug discovery, highlighting the limitations of current strategies, and exploring potential solutions using electro-mechano active polymer-based scaffolds based on conductive polymers. However, critical considerations such as the trade-off between 3D systems and nutrient exchange, biocompatibility, degradation, cell adhesion, longevity, and integration into wider systems must be carefully evaluated. Continued advancements in these areas will contribute to a better understanding of cardiac diseases, improved drug discovery, and the development of personalized treatment strategies for patients with cardiovascular disorders.

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Nanopillar/tube arrays have emerged as encouraging platforms, possessing remarkable advantages, including large specific areas and highly aligned orientations. Despite the progress of nano/microfabrication technologies, facile and controllable fabrication of conductive polymer nanopillar/tube arrays remains challenging. In this study, we demonstrate that the air-liquid interfacial self-assembly can be extended to obtain three-dimensional nanostructured arrays. A smart and novel method is proposed for preparing uniform conductive polymer nanopillar/tube arrays by a template-mediated interfacial synthesis approach. By utilizing capillary force, precise control processes of the nanostructure and patterned structure can be easily realized. Furthermore, a transfer strategy is devised, allowing for scalable fabrication and expansion of the applicability. Applications, including antibacterial surfaces and actuators, have been demonstrated. We extend the air-liquid interfacial synthesis technique as a powerful and universal strategy for producing ordered nanopillar/tube arrays and show the great potential of soft nanostructured arrays as advanced platforms in diverse applications.