NFC-enabled potentiostat and nitrocellulose-based metal electrodes for electrochemical lateral flow assay.

Rapid detection of pathogens at the point-of-need is crucial for preventing the spread of human, animal and plant diseases which can have devastating consequences both on the lives and livelihood of billions of people. Colorimetric, lateral flow assays consisting of a nitrocellulose membrane, are the preferred format today for low-cost on-site detection of pathogens. This assay format has, however, historically suffered from poor analytical performance and is not compatible with digital technologies. In this work, we report the development of a new class of digital diagnostics platform for precision point-of-need testing. This new versatile platform consists of two important innovations: i) A wireless and batteryless, microcontroller-based, low-cost Near Field Communication (NFC)-enabled potentiostat that brings high performance electroanalytical techniques (cyclic voltammetry, chronoamperometry, square wave voltammetry) to the field. The NFC-potentiostat can be operated with a mobile app by minimally trained users; ii) A new approach for producing nitrocellulose membranes with integrated electrodes that facilitate high performance electrochemical detection at the point-of-need. We produced an integrated system housed in a 3D-printed phone case and demonstrated its use for the detection of Maize Mosaic Virus (MMV), a plant pathogen, as a proof-of-concept application.

Disposable silicon-based all-in-one micro-qPCR for rapid on-site detection of pathogens.

Rapid screening and low-cost diagnosis play a crucial role in choosing the correct course of intervention when dealing with highly infectious pathogens. This is especially important if the disease-causing agent has no effective treatment, such as the novel coronavirus SARS-CoV-2, and shows no or similar symptoms to other common infections. Here, we report a disposable silicon-based integrated Point-of-Need transducer (TriSilix) for real-time quantitative detection of pathogen-specific sequences of nucleic acids. TriSilix can be produced at wafer-scale in a standard laboratory (37 chips of 10 × 10 × 0.65 mm in size can be produced in 7 h, costing ~0.35 USD per device). We are able to quantitatively detect a 563 bp fragment of genomic DNA of Mycobacterium avium subspecies paratuberculosis through real-time PCR with a limit-of-detection of 20 fg, equivalent to a single bacterium, at the 35th cycle. Using TriSilix, we also detect the cDNA from SARS-CoV-2 (1 pg) with high specificity against SARS-CoV (2003).

Paper-based platforms with coulometric readout for ascorbic acid determination in fruit juices.

There is growing interest in the development of simple, fast, sustainable and low-cost analytical methodologies on paper-based platforms. However, sensitive detection strategies that fit properly with these devices are still required. In this work, a calibration-free method is proposed for analytical determinations performed on paper-based electrochemical devices, in this case, for ascorbic acid. Carbon ink is deposited on a hydrophilic working area of the paper delimited with a hydrophobic wax. This maskless procedure is fast and cuts down ink waste. The connection of this working electrode to the potentiostat is provided by reusable gold-plated connector headers that provide also the reference and counter electrodes. The thickness of the paper substrate defines the electrochemical cell and confines a sample volume, ideal for thin-layer coulometry. Controlled-potential coulometry is performed applying a potential of +0.6 V for 50 s. The charge is calculated by measuring the area under the fast chronoamperogram and the concentration is determined following Faraday's law (known number of transferred electrons). This methodology was applied to the determination of ascorbic acid, with a limit of detection of 40 µM. Its concentration in commercial fruit juices can be directly determined in diluted samples. The absence of matrix effects is observed by comparing the results obtained before and after enzymatic reaction of the sample with cucumber ascorbate oxidase. Good accuracy and precision makes this method suitable for quality control of ascorbic acid in commercial juices. Underexploited coulometric readout can be applied as a fast (calibration-free) and low-cost (standards not required) transduction principle for the newly developed paper devices.

Monolithic Solder-On Nanoporous Si-Cu Contacts for Stretchable Silicone Composite Sensors.

We report a method of creating solderable, mechanically robust, electrical contacts to interface (soft) silicone-based strain sensors with conventional (hard) solid-state electronics using a nanoporous Si-Cu composite. The Si-based solder-on electrical contact consists of a copper-plated nanoporous Si top surface formed through metal-assisted chemical etching and electroplating and a smooth Si bottom surface that can be covalently bonded onto silicone-based strain sensors through plasma bonding. We investigated the mechanical and electrical properties of the contacts proposed under relevant ranges of mechanical stress for applications in physiological monitoring and rehabilitation. We also produced a series of proof-of-concept devices, including a wearable respiration monitor, leg band for exercise monitoring, and squeeze ball for monitoring rehabilitation of patients with hand injuries or neurological disorders to demonstrate the mechanical robustness and versatility of the technology developed in real-world applications.

Autocatalytic Metallization of Fabrics Using Si Ink, for Biosensors, Batteries and Energy Harvesting.

Commercially available metal inks are mainly designed for planar substrates (for example, polyethylene terephthalate foils or ceramics), and they contain hydrophobic polymer binders that fill the pores in fabrics when printed, thus resulting in hydrophobic electrodes. Here, a low-cost binder-free method for the metallization of woven and nonwoven fabrics is presented that preserves the 3D structure and hydrophilicity of the substrate. Metals such as Au, Ag, and Pt are grown autocatalytically, using metal salts, inside the fibrous network of fabrics at room temperature in a two-step process, with a water-based silicon particle ink acting as precursor. Using this method, (patterned) metallized fabrics are being enabled to be produced with low electrical resistance (less than 3.5 Ω sq-1). In addition to fabrics, the method is also compatible with other 3D hydrophilic substrates such as nitrocellulose membranes. The versatility of this method is demonstrated by producing coil antennas for wireless energy harvesting, Ag-Zn batteries for energy storage, electrochemical biosensors for the detection of DNA/proteins, and as a substrate for optical sensing by surface enhanced Raman spectroscopy. In the future, this method of metallization may pave the way for new classes of high-performance devices using low-cost fabrics.

In situ gold-nanoparticle electrogeneration on gold films deposited on paper for non-enzymatic electrochemical determination of glucose.

This work describes the development and evaluation of a new electrochemical platform based on the sustainable generation of gold-nanoparticles on paper-based gold-sputtered electrodes. The disposable porous paper electrode is combined with screen-printed electrodes for ensuring a precise electrogeneration of nanoparticles and also for the evaluation of these simple, versatile and low-cost microfluidic devices. Two types of chromatographic paper with different thicknesses have been evaluated. Paper gold working electrodes modified with gold nanoparticles were characterized by scanning electron microscopy and cyclic voltammetry using potassium ferrocyanide as a common redox probe, showing an improved electrochemical performance when compared to bare gold electrodes. The platform has been applied to the non-enzymatic determination of glucose, molecule of enormous interest. The porous gold structure made by sputtering on paper, modified with electrogenerated nanoparticles allowed precise and accurate determination of the analyte in beverages at low potential.

Electrogeneration of Gold Nanoparticles on Porous-Carbon Paper-Based Electrodes and Application to Inorganic Arsenic Analysis in White Wines by Chronoamperometric Stripping.

This paper describes the development of simple, sustainable, and low-cost strategies for signal enhancement on paper-based carbon platforms through gold nanoparticles electrogenerated from small volumes of tetrachloroauric (III) acid solutions. Carbon ink is deposited on a hydrophilic working area of the paper delimited with hydrophobic wax. This maskless procedure is fast and cuts down ink waste. The connection of this working electrode to the potentiostat is ensured with the use of screen-printed electrodes (SPEs). Close contact of the whole area of both carbon electrodes improves the precision of the nanostructuration. Resulting gold-modified paper-based carbon working electrodes (AuNPs-PCWEs) were characterized by cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), scanning electron microscopy (SEM), and electron dispersion X-ray spectrometry (SEM/EDX). This methodology was applied for the first time to the inorganic arsenic determination in commercial white wines by chronoamperometric stripping of the electrodeposited As(0). In an optimized system, As(III) was reduced and deposited as As(0) on the nanostructured surface by applying a potential of -0.3 V during 180 s. Then, anodic stripping chronoamperometry was performed at +0.4 V. The analytical signal was the current recorded at 30 s. On the other hand, As(V) was chemically reduced to As(III) with 0.2 M KI, and total determination of arsenic could be carried out. As(V) was determined as the difference between total As and As(III). Then, this fast, simple and low-cost method can be employed for speciation purposes. Limits of detection for As(III) and total arsenic (in the presence of KI) are 2.2 µg L-1 and 2.4 µg L-1, respectively, and indicate that this method is suitable for regulated quality control.

Integration of gold-sputtered electrofluidic paper on wire-included analytical platforms for glucose biosensing.

This work describes the fabrication and evaluation of an electroanalytical paper-based platform based on the combination of both, reusable and disposable materials in order to generate simple, versatile and low-cost microfluidic devices. With this aim, a holder containing metal wires that act as reusable reference and counter electrodes has been developed. The gold-sputtered paper electrode is disposable and easily interchangeable, meanwhile the platform that includes reference and counter electrodes can be reused. The detection zone in the paper is delimited by drawing a hydrophobic line with an inexpensive permanent marker. The effect of experimental variables such as adding solutions through the face where the gold was sputtered (upwards) or through the opposite one (downwards) as well as of other working parameters were studied by cyclic and differential pulse voltammetry with potassium ferrocyanide as a common redox probe and indicator species for enzymatic, immune and DNA biosensing. Enzymatic determination of glucose in real food samples prove the feasibility of the developed system for the construction of electrochemical biosensors.