Organic electrochemical transistors (OECTs) are the building blocks of biosensors, neuromorphic devices, and complementary circuits. One rule in the materials design for OECTs is the inclusion of a hydrophilic component in the chemical structure to enable ion transport in the film. Here, it is shown that the ladder-type, side-chain free polymer poly(benzimidazobenzophenanthro line) (BBL) performs significantly better in OECTs than the donor-acceptor type copolymer bearing hydrophilic ethylene glycol side chains (P-90). A combination of electrochemical techniques reveals that BBL exhibits a more efficient ion-to-electron coupling and higher OECT mobility than P-90. In situ atomic force microscopy scans evidence that BBL, which swells negligibly in electrolytes, undergoes a drastic and permanent change in morphology upon electrochemical doping. In contrast, P-90 substantially swells when immersed in electrolytes and shows moderate morphology changes induced by dopant ions. Ex situ grazing incidence wide-angle X-ray scattering suggests that the particular packing of BBL crystallites is minimally affected after doping, in contrast to P-90. BBL's ability to show exceptional mixed transport is due to the crystallites' connectivity, which resists water uptake. This side chain-free route for the design of mixed conductors could bring the n-type OECT performance closer to the bar set by their p-type counterparts.

The organic electrochemical transistor (OECT) is one of the most versatile bioelectronic devices. This review is a guide for how to characterize OECTs and monitor the mixed charge transport and swelling properties of the OECT channel materials.

Electrochemical detection of metabolites is essential for early diagnosis and continuous monitoring of a variety of health conditions. This review focuses on organic electronic material-based metabolite sensors and highlights their potential to tackle critical challenges associated with metabolite detection. We provide an overview of the distinct classes of organic electronic materials and biorecognition units used in metabolite sensors, explain the different detection strategies developed to date, and identify the advantages and drawbacks of each technology. We then benchmark state-of-the-art organic electronic metabolite sensors by categorizing them based on their application area (in vitro, bodyinterfaced, in vivo, and cell-interfaced). Finally, we share our perspective on using organic bioelectronic materials for metabolite sensing and address the current challenges for the devices and progress to come. CONTENTS 1. Introduction 4581 2. Metabolite Sensing in the Body at a Glance 4583 2.1. Metabolite Sensing and Signaling Mechanisms: Sensor−Transducer−Effector Model 4583 2.2. (Biological) Recognition Units 4584 3. Organic Electronic Materials in Metabolite Sensing 4588 3.1. Graphene 4588 3.2. Carbon Nanotubes 4590 3.3. Conjugated Polymers (CPs) 4590 3.4. Composite Materials 4591 4. Sensing Methods 4592 4.1. Electrodes 4593 4.1.1.

Among the existing two-dimensional materials, MXenes, i.e. transition metal carbides, nitrides and/or carbonitrides, stand out for their excellent electrochemical properties. Due to their high charge storage capacity, metal-like conductivity, biocompatibility as well as hydrophilicity, Ti3C2Tx MXene-based inks hold great potential for scalable production of skin conformable electronics via direct printing methods. Herein, we develop an aqueous MXene ink and inkjet-print MXene films on freestanding, flexible, and conducting polymer-based substrates. These skin-adherent MXene electrodes detect electrocardiography signals with high signal-to-noise ratio while exhibiting preserved electrical performance after 1000 cycles of bending with a 50 d long shelf life in ambient conditions. We show that printed MXene films can be further functionalized to perform as multifunctional biosensing units. When integrated with a sodium (Na+) ion selective membrane, MXene electrodes detect Na+ in artificial sweat with a sensitivity of 40 mV per decade. When the films are functionalized with antibodies, they generate an electrical signal in response to a pro-inflammatory cytokine protein (interferon gamma) with a sensitivity of 3.9 mV per decade. Our findings demonstrate how inkjet-printed MXene films simplify the fabrication of next-generation wearable electronic platforms that comprise multimodal sensors.

Poly(3,4-ethylenedioxythiophene) (PEDOT) doped with poly(styrene sulfonate) (PSS) is the most commonly used conducting polymer in organic bioelectronics. However, electrochemical capacitances exceeding the current state-of-the-art are required for enhanced transduction and stimulation of biological signals. The long-term stability of conducting polymer films during device operation and storage in aqueous environments remains a challenge for routine applications. In this work, we electrochemically synthesize a PEDOT composite comprising the water dispersible two-dimensional conducting material Ti3C2 MXene. We find that incorporating MXene as a co-dopant along with PSS leads to PEDOT:PSS:MXene films with remarkably high volumetric capacitance (607.0 ± 85.3 F cm−3) and stability (capacity retention = 78.44% ± 1.75% over 500 cycles), outperforming single dopant-comprising PEDOT films, i.e., PEDOT:PSS and PEDOT:MXene electropolymerized under the same conditions on identical surfaces. The stability of microfabricated PEDOT:PSS:MXene electrodes is evaluated under different conditions, i.e., when the films are exposed to sonication (∼100% retention over 6 min), upon immersion in cell culture media for 14 days (∆|Z| = 2.13%), as well as after continuous electrical stimulation. Furthermore, we demonstrate the use of a PEDOT:PSS:MXene electrode as an electrochemical sensor for sensitive detection of dopamine (DA). The sensor exhibited an enhanced electrocatalytic activity toward DA in a linear range from 1 µM to 100 μM validated in mixtures containing common interferents such as ascorbic acid and uric acid. PEDOT:PSS:MXene composite is easily formed on conductive substrates with various geometries and can serve as a high performance conducting interface for chronic biochemical sensing or stimulation applications.