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Organic mixed ionic‐electronic conductors (OMIECs) have emerged as promising materials for biological sensing, owing to their electrochemical activity, stability in an aqueous environment, and biocompatibility. Yet, OMIEC‐based sensors rely predominantly on the use of composite matrices to enable stimuli‐responsive functionality, which can exhibit issues with intercomponent interfacing. In this study, an approach is presented for non‐enzymatic glucose detection by harnessing a newly synthesized functionalized monomer, EDOT‐PBA. This monomer integrates electrically conducting and receptor moieties within a single organic component, obviating the need for complex composite preparation. By engineering the conditions for electrodeposition, two distinct polymer film architectures are developed: pristine PEDOT‐PBA and molecularly imprinted PEDOT‐PBA. Both architectures demonstrated proficient glucose binding and signal transduction capabilities. Notably, the molecularly imprinted polymer (MIP) architecture demonstrated faster stabilization upon glucose uptake while it also enabled a lower limit of detection, lower standard deviation, and a broader linear range in the sensor output signal compared to its non‐imprinted counterpart. This material design not only provides a robust and efficient platform for glucose detection but also offers a blueprint for developing selective sensors for a diverse array of target molecules, by tuning the receptor units correspondingly. [ABSTRACT FROM AUTHOR]

Electronic immunosensors are indispensable tools for diagnostics, particularly in scenarios demanding immediate results. Conventionally, these sensors rely on the chemical immobilization of antibodies onto electrodes. However, globular proteins tend to adsorb and unfold on these surfaces. Therefore, self‐assembled monolayers (SAMs) of thiolated alkyl molecules are commonly used for indirect gold–antibody coupling. Here, a limitation associated with SAMs is revealed, wherein they curtail the longevity of protein sensors, particularly when integrated into the state‐of‐the‐art transducer of organic bioelectronics—the organic electrochemical transistor. The SpyDirect method is introduced, generating an ultrahigh‐density array of oriented nanobody receptors stably linked to the gold electrode without any SAMs. It is accomplished by directly coupling cysteine‐terminated and orientation‐optimized spyTag peptides, onto which nanobody‐spyCatcher fusion proteins are autocatalytically attached, yielding a dense and uniform biorecognition layer. The structure‐guided design optimizes the conformation and packing of flexibly tethered nanobodies. This biolayer enhances shelf‐life and reduces background noise in various complex media. SpyDirect functionalization is faster and easier than SAM‐based methods and does not necessitate organic solvents, rendering the sensors eco‐friendly, accessible, and amenable to scalability. SpyDirect represents a broadly applicable biofunctionalization method for enhancing the cost‐effectiveness, sustainability, and longevity of electronic biosensors, all without compromising sensitivity. [ABSTRACT FROM AUTHOR]

The organic electrochemical transistor (OECT) is one of the most versatile building blocks within the bioelectronics device toolbox. While p‐type organic semiconductors have progressed as OECT channel materials, only a few n‐type semiconductors have been reported, precluding the development of advanced sensor‐integrated OECT‐based complementary circuits. Herein, green aldol polymerization is uses to synthesize lactone‐based n‐type conjugated polymers. Fluorination of the lactone‐based acceptor endows a fully locked backbone with a low‐lying lowest unoccupied molecular orbital, facilitating efficient ionic‐to‐electronic charge coupling. The resulting polymer has a record‐high n‐type OECT performance with a high product of mobility and capacitance (µC* = 108 F cm−1 V−1 s−1), excellent mobility (0.912 cm2 V−1 s−1), low threshold voltage (0.02 V), and fast switching speed (τON, τOFF = 336 µs,108 µs). This work demonstrates two types of device architectures and applications enabled by the high performance of this n‐type OECT, i.e., an artificial synapse and a complementary amplifier for detecting α‐synuclein, a potential biomarker of Parkinson's disease. This study shows that materials that enable high gain and fast speed n‐type OECTs can be developed via a green polymerization route, and the diverse form factors that these devices take promise for exploration of other application areas. [ABSTRACT FROM AUTHOR]

The recent emerging technologies (e.g., hybrid vehicles and wearable electronic devices) laid down critical and stringent considerations for their power sources. In this regard, supercapacitors (SCs) have become an attractive energy storage solution, thanks to their superior power density and stability over batteries. The continuous development of SCs is an active field of research toward practical application and commercialization. Yet, finding electrode materials with high capacitance, excellent cycle-life, and mechanical stability is of major interest to exceed the current state-of-the-art SCs. The unique set of features of conducting polymers (CPs), including remarkable electrochemical properties, tunable synthesis, solution-processable capabilities, and mechanical flexibility, promotes them at the forefront of materials for SCs electrodes. This review provides a comprehensive summary of CP-based SCs technology. We first start with a brief overview of CPs' unique properties and the principal synthetic methods that enable innovative fabrication. Then, a compact summary of the electrochemical and physicochemical characterization techniques is presented to assess the quality and mechanism of CP-based SCs. We limit our discussion to the published works in the last ten years. Finally, we highlight several research trends, key challenges, and opportunities of CP-based SCs for future research and development. [ABSTRACT FROM AUTHOR]

The first Telluride Science meeting (formerly TSRC) on organic mixed ionic and electronic conductors (OMIECs), Oct 3–7, 2022, brought together researchers across the field to understand the fundamental processes and identify out-standing questions related to this exciting class of materials. OMIECs are organic materials that promote the transport of mobile electronic charge carriers while simultaneously supporting ionic transport and ionic–electronic coupling. These properties open up broad areas of applications from energy to bioelectronics. Devices include batteries, supercapacitors, actuators, electrochromic displays, and organic electrochemical transistors (OECTs). They possess the key strengths of traditional organic electronic materials, such as synthetic tunability and low-temperature processing. Despite the recent advances in devices and applications achieved with such materials, many challenges and gaps in understanding remain. These topics hold the key to designing next-generation materials and devices that continue to push the limits of performance and stability and facilitate novel functionality. This perspective aims to summarize the current understanding, conversations, and debates that made this TSRC particularly engaging, enabling new directions and searching for missing pieces of the OMIEC puzzle. [ABSTRACT FROM AUTHOR]