Publications by authors named "Iuliana P Maria"

Introducing ethylene glycol (EG) side chains to a conjugated polymer backbone is a well-established synthetic strategy for designing organic mixed ion-electron conductors (OMIECs). However, the impact that film swelling has on mixed conduction properties has yet to be scoped, particularly for electron-transporting (n-type) OMIECs. Here, the authors investigate the effect of the length of branched EG chains on mixed charge transport of n-type OMIECs based on a naphthalene-1,4,5,8-tetracarboxylic-diimide-bithiophene backbone.

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Organic mixed ionic-electronic conductors (OMIECs) have varied performance requirements across a diverse application space. Chemically doping the OMIEC can be a simple, low-cost approach for adapting performance metrics. However, complex challenges, such as identifying new dopant materials and elucidating design rules, inhibit its realization.

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The tight regulation of the glucose concentration in the body is crucial for balanced physiological function. We developed an electrochemical transistor comprising an n-type conjugated polymer film in contact with a catalytic enzyme for sensitive and selective glucose detection in bodily fluids. Despite the promise of these sensors, the property of the polymer that led to such high performance has remained unknown, with charge transport being the only characteristic under focus.

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Electron-transporting (n-type) conjugated polymers have recently been applied in numerous electrochemical applications, where both ion and electron transport are required. Despite continuous efforts to improve their performance and stability, n-type conjugated polymers with mixed conduction still lag behind their hole-transporting (p-type) counterparts, limiting the functions of electrochemical devices. In this work, we investigate the effect of enhanced backbone coplanarity on the electrochemical activity and mixed ionic-electronic conduction properties of n-type polymers during operation in aqueous media.

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On-site signal amplification for bioelectronic sensing is a desirable approach to improving recorded signal quality and to reducing the burden on signal transmission and back-end electronics. While organic electrochemical transistors (OECTs) have been used as local transducers of bioelectronic signals, their current output presents challenges for implementation. OECT-based circuits offer new opportunities for high-performance signal processing.

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Conjugated polymers achieve redox activity in electrochemical devices by combining redox-active, electronically conducting backbones with ion-transporting side chains that can be tuned for different electrolytes. In aqueous electrolytes, redox activity can be accomplished by attaching hydrophilic side chains to the polymer backbone, which enables ionic transport and allows volumetric charging of polymer electrodes. While this approach has been beneficial for achieving fast electrochemical charging in aqueous solutions, little is known about the relationship between water uptake by the polymers during electrochemical charging and the stability and redox potentials of the electrodes, particularly for electron-transporting conjugated polymers.

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From established to emergent technologies, doping plays a crucial role in all semiconducting devices. Doping could, theoretically, be an excellent technique for improving repressively low transconductances in n-type organic electrochemical transistors - critical for advancing logic circuits for bioelectronic and neuromorphic technologies. However, the technical challenge is extreme: n-doped polymers are unstable in electrochemical transistor operating environments, air and water (electrolyte).

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Organic electrochemical transistors (OECTs) with high transconductance and good operating stability in an aqueous environment are receiving substantial attention as promising ion-to-electron transducers for bioelectronics. However, to date, in most of the reported OECTs, the fabrication procedures have been devoted to spin-coating processes that may nullify the advantages of large-area and scalable manufacturing. In addition, conventional microfabrication and photolithography techniques are complicated or incompatible with various nonplanar flexible and curved substrates.

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A promising class of materials for applications that rely on electron transfer for signal generation are the n-type semiconducting polymers. Here we demonstrate the integration of an n-type conjugated polymer with a redox enzyme for the autonomous detection of glucose and power generation from bodily fluids. The reversible, mediator-free, miniaturized glucose sensor is an enzyme-coupled organic electrochemical transistor with a detection range of six orders of magnitude.

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Conjugated polymers are promising engineering tools for establishing bilateral electrical communication with living systems. The free energy of their films, the roughness, and charge density play major roles in determining their interactions with lipid bilayers, which form the membrane barrier around every living cell allowing for molecular exchange with the extracellular environment. In this work, we investigate lipid bilayer formation from synthetic lipid vesicles (liposomes) on a series of amphiphilic copolymer films based on naphthalene 1,4,5,8 tetracarboxylic diimide bithiophene (NDI-T2) backbone where the alkyl side chain is gradually exchanged for an ethylene glycol-based side chain.

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With a host of new materials being investigated as active layers in organic electrochemical transistors (OECTs), several advantageous characteristics can be utilized to improve transduction and circuit level performance for biosensing applications. Here, the subthreshold region of operation of one recently reported high performing OECT material, poly(2-(3,3'-bis(2-(2-(2-methoxyethoxy)ethoxy)ethoxy)-[2,2'-bithiophen]-5-yl)thieno[3,2-]thiophene), p(g2T-TT) is investigated. The material's high subthreshold slope (SS) is exploited for high voltage gain and low power consumption.

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Article Synopsis
  • Enzymes are highly specific and reversible, making them ideal for use as biorecognition elements in biosensors to detect various metabolites, including lactate, which is important in health contexts.
  • The study presents a novel all-polymer micrometer-scale transistor platform that enhances enzyme-electrode interaction, allowing for faster, more sensitive detection without the need for complex mediators.
  • This new device improves upon traditional amperometric sensors by amplifying signals and simplifying the design, paving the way for advancements in both biosensing and enzyme-based energy technologies.
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We report a design strategy that allows the preparation of solution processable n-type materials from low boiling point solvents for organic electrochemical transistors (OECTs). The polymer backbone is based on NDI-T2 copolymers where a branched alkyl side chain is gradually exchanged for a linear ethylene glycol-based side chain. A series of random copolymers was prepared with glycol side chain percentages of 0, 10, 25, 50, 75, 90, and 100 with respect to the alkyl side chains.

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