Reversible modulation of the redox activity in conducting polymer nanofilms induced by hydrophobic collapse of a surface-grafted polyelectrolyte

Fenoy, Gonzalo E.; Giussi, Juan M.; Bilderling, Catalina von; Maza, Eliana; Pietrasanta, Lı́a I.; Knoll, Wolfgang; Marmisollé, Waldemar A.; Azzaroni, Omar

doi:10.1016/j.jcis.2018.02.014

Cited by 21 publications

(36 citation statements)

References 50 publications

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“…[ 49–52 ] Typically, when the electrode surface is rough, the charging/discharging features of the interface cannot be precisely described with a capacitive element, and a CPE is employed. [ 48 ] The impedance of the CPE is described by Z CPE = Yo −1 ( jω ) − n , and the magnitude of the deviation from the capacitive behavior is defined by n . When 0.8 < n < 1, the CPE can be considered as a capacitance.…”

Section: Resultsmentioning

confidence: 99%

“…[44,47] While several circuits have been developed for conducting polymer electrodes, and particularly www.advelectronicmat.de for PEDOT:PSS, the interpretation of the EIS response of conducting polymers is not simple. [48] Figure 5A shows a schematic picture of the charge transport processes that take place, whereas a more detailed description of the EIS model can be found in Supporting Information.…”

Section: Electrochemical Impedance Spectroscopy Characterizationmentioning

confidence: 99%

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PEDOT:Tosylate‐Polyamine‐Based Organic Electrochemical Transistors for High‐Performance Bioelectronics

Fenoy

Bilderling

Knoll

et al. 2021

Adv Elect Materials

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The construction of organic electrochemical transistors (OECTs) using poly(3,4‐ethylenedioxythiophene):tosylate and polyallylamine hydrochloride composites as conducting channel material is presented. The regulation of the polyelectrolyte‐to‐conducting polymer proportion allows one to easily tune both electronic and ionic characteristics of the transistors, yielding devices with low threshold voltages while preserving high transconductance, which is an essential requisite for the effective integration of OECTs with biological systems. Also, the incorporation of the polyelectrolyte enhances the transient response of the OECTs during the ON/OFF switching, probably due to improved ion transport. Furthermore, the integration of pH‐sensitive amino moieties not only improves the pH response of the transistors but also allows for the non‐denaturing electrostatic anchoring of functional enzymes. As a proof‐of‐concept, acetylcholinesterase is electrostatically immobilized by taking advantage of the NH2 moieties, and the OECTs‐based sensors are able to successfully monitor the neurotransmitter acetylcholine in the range 5–125 µm.

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Section: Resultsmentioning

confidence: 99%

Section: Electrochemical Impedance Spectroscopy Characterizationmentioning

confidence: 99%

PEDOT:Tosylate‐Polyamine‐Based Organic Electrochemical Transistors for High‐Performance Bioelectronics

Fenoy

Bilderling

Knoll

et al. 2021

Adv Elect Materials

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“…Polymer brushes are assemblies of macromolecules that are tethered by one end to a surface. These macromolecular architectures bearing different functional groups along their backbones can be grafted on different surfaces, and even in constrained environments . There are two main strategies for generating polymer brushes on solid surfaces: “grafting to” and “grafting from.” In the “grafting‐to” technique, presynthesized polymers are anchored to a surface from solution.…”

Section: Functionalization Of Solid‐state Nanoporesmentioning

confidence: 99%

Molecular Design of Solid‐State Nanopores: Fundamental Concepts and Applications

et al. 2019

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Solid‐state nanopores are fascinating objects that enable the development of specific and efficient chemical and biological sensors, as well as the investigation of the physicochemical principles ruling the behavior of biological channels. The great variety of biological nanopores that nature provides regulates not only the most critical processes in the human body, including neuronal communication and sensory perception, but also the most important bioenergetic process on earth: photosynthesis. This makes them an exhaustless source of inspiration toward the development of more efficient, selective, and sophisticated nanopore‐based nanofluidic devices. The key point responsible for the vibrant and exciting advance of solid nanopore research in the last decade has been the simultaneous combination of advanced fabrication nanotechnologies to tailor the size, geometry, and application of novel and creative approaches to confer the nanopore surface specific functionalities and responsiveness. Here, the state of the art is described in the following critical areas: i) theory, ii) nanofabrication techniques, iii) (bio)chemical functionalization, iv) construction of nanofluidic actuators, v) nanopore (bio)sensors, and vi) commercial aspects. The plethora of potential applications once envisioned for solid‐state nanochannels is progressively and quickly materializing into new technologies that hold promise to revolutionize the everyday life.

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“…The reduced graphene oxide field-effect transistors (rGO FETs) were prepared from interdigitated electrodes as we described in previous works. 16,42 Poly [ 2) Acylation of amine modified rGO-FETs with α-bromoisobutyryl bromide to obtain ATRP initiators sites: 43 The amine modified rGO-FETs substrates were immersed in an Erlenmeyer containing 40 mL of dry THF and 2 mL of triethylamine under N 2 . After this, the reaction solution was placed in an ice bath and 2 mL of αbromoisobutyryl bromide was added slowly using a pressure-equalizing dropping funnel.…”

Section: Graphene-based Transistor Fabricationmentioning

confidence: 99%

Reversible Switching of the Dirac Point in Graphene Field-Effect Transistors Functionalized with Responsive Polymer Brushes

et al. 2019

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The reversible control of the graphene Dirac point using external chemical stimuli is of major interest in the development of advanced electronic devices such as sensors and smart logic gates. Here, we report the coupling of chemo-responsive polymer brushes to reduced graphene oxide (rGO) based field-effect transistors (FETs) to modulate the graphene Dirac point in the presence of specific divalent cations. Poly[2-(methacryloyloxy)ethyl]phosphate (PMEP) brushes were grown on the transistor channel by atom transfer radical polymerization (ATRP) initiated from amine-pyrene linkers non-covalently attached to rGO surfaces. Our results show an increase in the Dirac point voltage, due to electrostatic gating effects, upon the specific binding of Ca 2+ and Mg 2+ to the PMEP brushes. We demonstrate that the electrostatic gating is reversibly controlled by the charge density of the polymer brushes, which depends on the divalent cation concentration. Moreover, a theoretical formalism based on the Grahame equation and a Langmuir-type binding isotherm is presented to obtain the PMEP-cation association constant from the experimental data.

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Reversible modulation of the redox activity in conducting polymer nanofilms induced by hydrophobic collapse of a surface-grafted polyelectrolyte

Cited by 21 publications

References 50 publications

PEDOT:Tosylate‐Polyamine‐Based Organic Electrochemical Transistors for High‐Performance Bioelectronics

PEDOT:Tosylate‐Polyamine‐Based Organic Electrochemical Transistors for High‐Performance Bioelectronics

Molecular Design of Solid‐State Nanopores: Fundamental Concepts and Applications

Reversible Switching of the Dirac Point in Graphene Field-Effect Transistors Functionalized with Responsive Polymer Brushes

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