An electrochemical impedance spectroscopy (EIS) sensor design is proposed based on a standard interdigitated electrode layout in which the smaller working electrode consists of gold (Au) whereas the larger combined counter and reference electrode is coated with a porous layer of polypyrrole (PPy) doped with polystyrene sulfonate (PSS) (PPy : PSS). Each electrode material was first characterized by EIS in a standard 3‐electrode setup with subsequent spectra fitting by a modified Randles equivalent circuit. The differences in the spectra obtained by the PPy : PSS coated electrodes can be explained by an increased electroactive surface area due to the porous polymer film. The changes in morphology of the film are discussed with respect to the evolution of the elements of the electric equivalent circuit. When applying the Au/PPy : PSS electrode combination to a standard 2‐electrode arrangement, the enlarged highly electroactive surface area of the PPy : PSS coating lowers the interfacial impedance in a way that mainly the gold working electrode contributes to the overall system impedance. Therefore, obtaining reproducible EIS signals depends only on the electrode's open‐circuit potential (OCP) and on additional adsorption events at the gold electrode/electrolyte interface. We present a protocol for microelectrode coating with PPy : PSS, which enables highly stable 2‐electrode EIS experiments without the need of a reference electrode. This combination is believed to be very useful if an integration of sensing electrodes inside Micro Total Analysis Systems is aspired.
Two-dimensional (2D) materials, such as graphene, are seen as potential candidates for fabricating electronic devices and circuits on flexible substrates. Inks or dispersions of 2D materials can be deposited on flexible substrates by large-scale coating techniques, such as inkjet printing and spray coating. One of the main issues in coating processes is nonuniform deposition of inks, which may lead to large variations of properties across the substrates. Here, we investigate the role of surface morphology on the performance of graphene ink deposited on different paper substrates with specific top coatings. Substrates with good wetting properties result in reproducible thin films and electrical properties with low sheet resistance. The correct choice of surface morphology enables high-performance films without postdeposition annealing or treatment. Scanning terahertz time-domain spectroscopy (THz-TDS) is introduced to evaluate both the uniformity and the local conductivity of graphene inks on paper. A paper-based strain gauge is demonstrated and a variable resistor acts as an on–off switch for operating an LED. Customized surfaces can thus help in unleashing the full potential of ink-based 2D materials.
A novel electrochemical impedance spectroscopy (EIS) sensor design, based on a standard interdigitated electrode arrangement in which the working electrode consists of gold and the combined counter and reference electrodes of polypyrrole doped with polystyrene sulfonate (PPy:PSS), is evaluated for biosensing applications. The performance is successfully proved by immobilization of a thiolated biotin as a self‐assembled monolayer (SAM), followed by streptavidin and a biotinylated horseradish peroxidase. It is shown that specific binding of biomolecules takes place only at the gold electrode. The binding activities are not influenced by the addition of small amounts of the nonionic surfactant Pluronic F‐68. The immobilization process is monitored online with EIS showing an excellent repeatability of the EIS signals in comparison with Au–Au electrode configuration even after electrode regeneration.
Electrowetting-on-dielectric is a decent technique to manipulate discrete volumes of liquid in form of droplets. In the last decade, electrowetting-on-dielectric systems, also called digital microfluidic systems, became more frequently used for a variety of applications because of their high flexibility and reconfigurability. Thus, one design can be adapted to different assays by only reprogramming. However, this flexibility can only be useful if the entire system is portable and easy to use. This paper presents the development of a portable, standalone digital microfluidic system based on a Linux-based operating system running on a Raspberry Pi, which is unique. We present "PortaDrop" exhibiting the following key features: (1) an "all-in-one box" approach, (2) a user-friendly, self-explaining graphical user interface and easy handling, (3) the ability of integrated electrochemical measurements, (4) the ease to implement additional lab equipment via Universal Serial Bus and the General Purpose Interface Bus as well as (5) a standardized experiment documentation. We propose that PortaDrop can be used to carry out experiments in different applications, where small sample volumes in the nanoliter to picoliter range need to be handled an analyzed automatically. As a first application, we present a protocol, where a droplet is consequently exchanged by droplets of another medium using passive dispensing. The exchange is monitored by electrical impedance spectroscopy. It is the first time, the media exchange caused by passive dispensing is characterized by electrochemical impedance spectroscopy. Summarizing, PortaDrop allows easy combination of fluid handling by means of electrowetting and additional sensing.
A stable reference electrode (RE) plays a crucial role in the performance of an ion-sensitive field-effect transistor (ISFET) for bio/chemical sensing applications. There is a strong demand for the miniaturization of the RE for integrated sensor systems such as lab-on-a-chip (LoC) or point-of-care (PoC) applications. Out of several approaches presented so far to integrate an on-chip electrode, there exist critical limitations such as the effect of analyte composition on the electrode potential and drifts during the measurements. In this paper, we present a micro-scale solid-state pseudo-reference electrode (pRE) based on poly(3,4-ethylene dioxythiophene): poly(styrene sulfonic acid) (PEDOT:PSS) coated with graphene oxide (GO) to deploy with an ion-sensitive field-effect transistor (ISFET)-based sensor platform. The PEDOT:PSS was electropolymerized from its monomer on a micro size gold (Au) electrode and, subsequently, a thin GO layer was deposited on top. The stability of the electrical potential and the cross-sensitivity to the ionic strength of the electrolyte were investigated. The presented pRE exhibits a highly stable open circuit potential (OCP) for up to 10 h with a minimal drift of ~0.65 mV/h and low cross-sensitivity to the ionic strength of the electrolyte. pH measurements were performed using silicon nanowire field-effect transistors (SiNW-FETs), using the developed pRE to ensure good gating performance of electrolyte-gated FETs. The impact of ionic strength was investigated by measuring the transfer characteristic of a SiNW-FET in two electrolytes with different ionic strengths (1 mM and 100 mM) but the same pH. The performance of the PEDOT:PSS/GO electrode is similar to a commercial electrochemical Ag/AgCl reference electrode.
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