Microelectrode arrays (MEAs) are widely used platforms in bioelectronics to study electrogenic cells. In recent years, the processing of conductive polymers for the fabrication of three-dimensional electrode arrays has gained increasing interest for the development of novel sensor designs. Here, additive manufacturing techniques are promising tools for the production of MEAs with three-dimensional electrodes. In this work, a facile additive manufacturing process for the fabrication of MEAs that feature needle-like electrode tips, so-called μ-needles, is presented. To this end, an aerosol-jet compatible PEDOT:PSS and multiwalled carbon nanotube composite ink with a conductivity of 323 ± 75 S m −1 is developed and used in a combined inkjet and aerosol-jet printing process to produce the μ-needle electrode features. The μ-needles are fabricated with a diameter of 10 ± 2 μm and a height of 33 ± 4 μm. They penetrate an inkjet-printed dielectric layer to a height of 12 ± 3 μm. After successful printing, the electrochemical properties of the devices are assessed via cyclic voltammetry and impedance spectroscopy. The μ-needles show a capacitance of 242 ± 70 nF at a scan rate of 5 mV s −1 and an impedance of 128 ± 22 kΩ at 1 kHz frequency. The stability of the μ-needle MEAs in aqueous electrolyte is demonstrated and the devices are used to record extracellular signals from cardiomyocyte-like HL-1 cells. This proof-of-principle experiment shows the μ-needle MEAs' cell-culture compatibility and functional integrity to investigate electrophysiological signals from living cells.
Stochastic impact electrochemistry is a promising concept to detect ultralow concentrations of nanoparticles in solution. However, statistically reliable sensor outputs require an appropriate number of observed nanoparticle collision events. Here, arrays of individually addressable electrodes allow increasing the effective detection area, and thereby the number of collision events, without sacrificing the signal-to-noise ratio. At the same time, however, these measurements typically increase the surface-to-volume ratio of the system, leading to a stronger influence of adsorption on the number of available particles. We address this issue of nanoparticle adsorption by controlling the electrode–electrolyte interface close to the detection electrodes. We use a direct nanoimpact experiment to demonstrate that a negatively charged surface leads to electrostatic repulsion, which results in a 2.5-fold increase in the number of detected collision events. Adding to this improved sensor performance, a tunable shield electrode offers a versatile tool to study nanoparticle adsorption at the solid–liquid interface.
Recent investigations into cardiac or nervous tissues call for systems that are able to electrically record in 3D as opposed to 2D. Typically, challenging microfabrication steps are required to produce 3D microelectrode arrays capable of recording at the desired position within the tissue of interest. As an alternative, additive manufacturing is becoming a versatile platform for rapidly prototyping novel sensors with flexible geometric design. In this work, 3D MEAs for cell-culture applications were fabricated using a piezoelectric inkjet printer. The aspect ratio and height of the printed 3D electrodes were user-defined by adjusting the number of deposited droplets of silver nanoparticle ink along with a continuous printing method and an appropriate drop-to-drop delay. The Ag 3D MEAs were later electroplated with Au and Pt in order to reduce leakage of potentially cytotoxic silver ions into the cellular medium. The functionality of the array was confirmed using impedance spectroscopy, cyclic voltammetry, and recordings of extracellular potentials from cardiomyocyte-like HL-1 cells.
Microfluidic paper-based analytical devices (μPADs) have experienced an unprecedented story of success. In particular, as of today, most people have likely come into contact with one of their two most famous examplesthe pregnancy or the SARS-CoV-2 antigen test. However, their sensing performance is constrained by the optical readout of nanoparticle agglomeration, which typically allows only qualitative measurements. In contrast, single-impact electrochemistry offers the possibility to quantify species concentrations beyond the pM range by resolving collisions of individual species on a microelectrode. Within this work, we investigate the integration of stochastic sensing into a μPAD design by combining a wax-patterned microchannel with a microelectrode array to detect silver nanoparticles (AgNPs) by their oxidative dissolution. In doing so, we demonstrate the possibility to resolve individual nanoparticle collisions in a reference-on-chip configuration. To simulate a lateral flow architecture, we flush previously dried AgNPs along a microchannel toward the electrode array, where we are able to record nanoparticle impacts. Consequently, single-impact electrochemistry poses a promising candidate to extend the limits of lateral flow-based sensors beyond current applications toward a fast and reliable detection of very dilute species on site.
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