Prussian Blue (PB) is commonly incorporated into screen-printed enzymatic devices since it enables the determination of the enzymatically produced hydrogen peroxide at low potentials. Inkjet printing is gaining popularity in the development of electrochemical sensors as a substitute for screen printing. This work presents a fully inkjet-printed graphene–Prussian Blue platform, which can be paired with oxidase enzymes to prepare a biosensor of choice. The graphene electrode was inkjet-printed on a flexible polyimide substrate and then thermally and photonically treated with intense pulsed light, followed by inkjet printing of a PB nanoparticle suspension. The optimization of post-printing treatment and electrode deposition conditions was performed to yield a platform with minimal sheet resistance and peak potential differences. A thorough study of PB deposition was conducted: the fully inkjet-printed system was compared against sensors with PB deposited chemically or by drop casting the PB suspension on different kinds of carbon electrodes (glassy carbon, commercial screen-printed, and in-house inkjet-printed electrodes). For hydrogen peroxide detection, the fully inkjet-printed platform exhibits excellent sensitivity, a wider linear range, better linearity, and greater stability towards higher concentrations of peroxide than the other tested electrodes. Finally, lactate oxidase was immobilized in a chitosan matrix, and the prepared biosensor exhibited analytical performance comparable to other lactate sensors found in the literature in a wide, physiologically relevant linear range for measuring lactate concentration in sweat. The development of mediator-modified electrodes with a single fabrication technology, as demonstrated here, paves the way for the scalable production of low-cost, wearable, and flexible biosensors.

Reliable models of the lung environment are important for research on inhalation products, drug delivery, and how aerosols interact with tissue. pH fluctuations frequently accompany real physiological processes in pulmonary environments, so monitoring pH changes in lung-on-a-chip devices is of considerable relevance. Presented here are flexible, miniaturized, inkjet-printed pH sensors that have been developed with the aim of integration into lung-on-a-chip systems. Different types of functional pH-sensitive materials were tested: hydrogen-selective plasticized PVC membranes and polyaniline (both electrodeposited and dropcast). Their deposition and performance were evaluated on different flexible conducting substrates, including screen-printed carbon electrodes (SPE) and inkjet-printed graphene electrodes (IJP-Gr). Finally, a biocompatible dropcast polyaniline-modified IJP was selected and paired with an inkjet-printed Ag/AgCl quasireference electrode. The printed potentiometric device showed Nernstian sensitivity (58.8 mV/pH) with good reproducibility, reversibility, and potential stability. The optimized system was integrated with a developed lung-on-a-chip model with an electrospun polycaprolactone membrane and alginate, simulating the alveolar barrier and the natural mucosal environment, respectively. The permeability of the system was studied by monitoring the pH changes upon the introduction of a 10 wt.% acetic acid aerosol. Overall, the presented approach shows that electrospun-hydrogel materials together with integrated microsensors can help create improved models for studying aerosol transport, diffusion, and chemically changing environments that are relevant for inhalation therapy and respiratory research. These results show that our system can combine mechanical behavior with chemical sensing in one platform, which may be useful for future development of lung-on-a-chip technologies.

Using disposable screen-printed electrodes faces major challenges when attempting to monitor a continuous process, especially in systems where there is pronounced adsorption, fouling, degradation, or in cases of irreversible electrochemical reactions. Methylene Blue (MB) exhibits some therapeutic properties and is commonly used as a redox reporter in DNA sensors, but is also considered a toxic pollutant in aquatic systems. MB demonstrates strong adsorption to carbon materials, which prevents its electroanalytical determination in multiple measurements with a single electrode. Our work details direct electrochemical determination of MB with only the native carbon screen-printed working electrode as sensing material and optimization of the analytical method. In batch mode, we significantly improved sensitivity and interelectrode reproducibility by introducing a prepolarization step, but successive measurements in lower concentrations were not feasible due to strong adsorption. A fully customizable, modular flow cell was 3D printed to allow in operando replacement of the planar screen-printed three-electrode system after measurement during continuous flow. As confirmed by mechanical properties testing, the rigid polyacrylate upper section of the flow cell provides structural stability, combined with a flexible TPU lower section which enables effortless sensor hot swapping and effective sealing during flow. With an optimized hot swapping flow detection method, MB was detected via square wave voltammetry with a sensitivity of 65.59 µA/µM and a calculated LOD of 7.75 nM, which outperforms similar systems from the literature. We envisage this approach can be integrated into low-cost continuous environmental monitoring systems or in-line quality control, especially in flow chemistry synthesis.