The Influence of Microstructure on TCR for Inkjet-Printed Resistive Temperature Detectors Fabricated Using AgNO3/Ethylene-Glycol-Based Inks.

This study investigated the influence of microstructure on the performance of Ag inkjet-printed, resistive temperature detectors (RTDs) fabricated using particle-free inks based on a silver nitrate (AgNO3) precursor and ethylene glycol as the ink solvent. Specifically, the temperature coefficient of resistance (TCR) and sensitivity for sensors printed using inks that use monoethylene glycol (mono-EG), diethylene glycol (di-EG), and triethylene glycol (tri-EG) and subjected to a low-pressure argon (Ar) plasma after printing were investigated. Scanning electron microscopy (SEM) confirmed previous findings that microstructure is strongly influenced by the ink solvent, with mono-EG inks producing dense structures, while di- and tri-EG inks produce porous structures, with tri-EG inks yielding the most porous structures. RTD testing revealed that sensors printed using mono-EG ink exhibited the highest TCR (1.7 × 10-3/°C), followed by di-EG ink (8.2 × 10-4/°C) and tri-EG ink (7.2 × 10-4/°C). These findings indicate that porosity exhibits a strong negative influence on TCR. Sensitivity was not strongly influenced by microstructure but rather by the resistance of RTD. The highest sensitivity (0.84 Ω/°C) was observed for an RTD printed using mono-EG ink but not under plasma exposure conditions that yield the highest TCR.

Soft implantable printed bioelectronic system for wireless continuous monitoring of restenosis.

Atherosclerosis is a prominent cause of coronary artery disease and broader cardiovascular diseases, the leading cause of death worldwide. Angioplasty and stenting is a common treatment, but in-stent restenosis, where the artery re-narrows, is a frequent complication. Restenosis is detected through invasive procedures and is not currently monitored frequently for patients. Here, we report an implantable vascular bioelectronic device using a newly developed miniaturized strain sensor via microneedle printing methods. A capillary-based printing system achieves high-resolution patterning of a soft, capacitive strain sensor. Ink and printing parameters are evaluated to create a fully printed sensor, while sensor design and sensing mechanism are studied to enhance sensitivity and minimize sensor size. The sensor is integrated with a wireless vascular stent, offering a biocompatible, battery-free, wireless monitoring system compatible with conventional catheterization procedures. The vascular sensing system is demonstrated in an artery model for monitoring restenosis progression. Collectively, the artery implantable bioelectronic system shows the potential for wireless, real-time monitoring of various cardiovascular diseases and stent-integrated sensing/treatments.

3D Bioprinting for Vascularization.

In the world of clinic treatments, 3D-printed tissue constructs have emerged as a less invasive treatment method for various ailments. Printing processes, scaffold and scaffold free materials, cells used, and imaging for analysis are all factors that must be observed in order to develop successful 3D tissue constructs for clinical applications. However, current research in 3D bioprinting model development lacks diverse methods of successful vascularization as a result of issues with scaling, size, and variations in printing method. This study analyzes the methods of printing, bioinks used, and analysis techniques in 3D bioprinting for vascularization. These methods are discussed and evaluated to determine the most optimal strategies of 3D bioprinting for successful vascularization. Integrating stem and endothelial cells in prints, selecting the type of bioink according to its physical properties, and choosing a printing method according to physical properties of the desired printed tissue are steps that will aid in the successful development of a bioprinted tissue and its vascularization.

Design, Fabrication, and Optimization of a Printed Ag Nanoparticle-Based Flexible Capacitive Sensor for Automotive IVI Bezel Display Applications.

Since printed capacitive sensors provide better sensing performance, they can be used in automotive bezel applications. It is necessary to fabricate such sensors and apply an optimization approach for choosing the optimal sensor pattern. In the present work, an effort was made to formulate interdigitated pattern-printed Silver (Ag) electrode flexible sensors and adopt the Taguchi Grey Relational (TGR)-based optimization approach to enhance the flexible sensor's panel for enhanced automobile infotainment applications. The optimization technique was performed to derive better design considerations and analyze the influence of the sensor's parameters on change in capacitance when touched and production cost. The fabricated flexible printed sensors can provide better sensing properties. A design pattern which integrates an overlap of 15 mm, an electrode line width of 0.8 mm, and an electrode gap 0.8 mm can produce a higher change in capacitance and achieve a lower weight. The overlap has a greater influence on sensor performance owing to its optimization of spatial interpolation.

Implementation of 3D printing technologies to electrochemical and optical biosensors developed for biomedical and pharmaceutical analysis.

Three-dimensional (3D) printing technology has been applied in many areas. In recent years, new generation biosensors have been emerged with the progress on 3D printing technology (3DPT). Especially in the development of optical and electrochemical biosensors, 3DPT provides many advantages such as low cost, easy to manufacturing, being disposable and allow point of care testing. In this review, recent trends in the development of 3DPT based electrochemical and optical biosensors with their applications in the field of biomedical and pharmaceutical are examined. In addition, the advantages, disadvantages and future opportunities of 3DPT are discussed.

Cold Atmospheric Plasma-Assisted Direct Deposition of Polypyrrole-Ag Nanocomposites for Flexible Electronic Sensors.

Conductive polymers and their composite materials have attracted considerable interest due to their potential applications in sensors, actuators, drug delivery systems, and energy storage devices. Despite their wide range of applications, many challenges remain primarily with respect to the complex synthesis and time-consuming manufacturing steps that are often required in the fabrication process of various devices with conductive polymers. Here, we demonstrate the novel use of cold atmospheric plasma (CAP)-assisted deposition technologies as a solvent-free and scalable approach for in situ polymerization and direct deposition of conductive polypyrrole-silver (PPy-Ag) nanocomposites onto the desired substrates under atmospheric conditions. In this study, a systematic approach with different precursor composition mixtures containing pyrrole as the monomer and AgNO3 as the photoinitiator was investigated to assess the effect of precursor composition on the final chemical, electrical, and mechanical properties of the PPy-Ag nanocomposite thin-film coatings which were characterized by scanning electron microscopy, Fourier transform infrared spectroscopy, X-ray diffraction, and cyclic bending tests. The characterizations indicated the possibility of fabricating PPy-Ag nanocomposite films with tunable degrees of polymerization and Ag nanoparticle loading by simply varying the percentage of AgNO3 in precursor composition mixtures. Finally, as a proof of concept, the potential use of the PPy-Ag nanocomposite films with different Ag nanoparticle loading percentages was assessed for humidity sensing by measuring their level of change in electrical resistance in the relative humidity range of 12-60%. It is envisioned that the developed CAP-assisted deposition technology can provide a new stepping stone toward scalable additive manufacturing of various functional nanocomposite films for different low-cost and flexible electronic applications.

New carbon black-based conductive filaments for the additive manufacture of improved electrochemical sensors by fused deposition modeling.

The development of a homemade carbon black composite filament with polylactic acid (CB-PLA) is reported. Optimized filaments containing 28.5% wt. of carbon black were obtained and employed in the 3D printing of improved electrochemical sensors by fused deposition modeling (FDM) technique. The fabricated filaments were used to construct a simple electrochemical system, which was explored for detecting catechol and hydroquinone in water samples and detecting hydrogen peroxide in milk. The determination of catechol and hydroquinone was successfully performed by differential pulse voltammetry, presenting LOD values of 0.02 and 0.22 µmol L-1, respectively, and recovery values ranging from 91.1 to 112% in tap water. Furthermore, the modification of CB-PLA electrodes with Prussian blue allowed the non-enzymatic amperometric detection of hydrogen peroxide at 0.0 V (vs. carbon black reference electrode) in milk samples, with a linear range between 5.0 and 350.0 mol L-1 and low limit of detection (1.03 µmol L-1). Thus, CB-PLA can be successfully applied as additively manufactured electrochemical sensors, and the easy filament manufacturing process allows for its exploration in a diversity of applications.

Fabrication of Low-Cost Resistance Temperature Detectors and Micro-Heaters by Electrohydrodynamic Printing.

EHD printing is an advanced deposition technology that is commonly utilized for the direct manufacture of electrical devices. In this study, meander-type resistive electrodes consisting of silver nanoparticles were printed directly on rigid glass and flexible polyethylene terephthalate (PET) substrates. High-resolution patterns of ≈50 µm linewidth were successfully printed on untreated surfaces utilizing a bigger nozzle of 100 µm inner diameter after improving the experimental settings. The manufactured electrodes were evaluated and used as Resistance Temperature Detectors (RTDs) and micro-heaters in a systematic manner. The temperature sensors performed well, with a Temperature Coefficient of Resistivity (TCRs) of 11.5 ×10-3/°C and 13.3 ×10-3/°C, for glass and PET substrates, respectively, throughout a wide temperature range of 100 °C and 90 °C. Furthermore, the RTDs had a quick response and recovery time, as well as minimal hysteresis. The electrodes' measured sensitivities as micro-heaters were 3.3 °C/V for glass and 6.8 °C/V for PET substrates, respectively. The RTDs were utilized for signal conditioning in a Wheatstone bridge circuit with a self-heating temperature of less than 1 °C as a practical demonstration. The micro-heaters have a lot of potential in the field of soft wearable electronics for biomedical applications, while the extremely sensitive RTDs have a lot of potential in industrial situations for temperature monitoring.

Critical Salt Loading in Flexible Poly(vinyl alcohol) Sensors Fabricated by an Inkjet Printing and Plasma Reduction Method.

We report a low-temperature inkjet printing and plasma treatment method using silver nitrate ink that allows the fabrication of conductive silver traces on poly(vinyl alcohol) (PVA) film with good fidelity and without degrading the polymer substrate. In doing so, we also identify a critical salt loading in the film that is necessary to prevent the polymer from reacting with the silver nitrate-based ink, which improves the resolution of the silver trace while simultaneously lowering its sheet resistance. Silver lines printed on PVA film using this method have sheet resistances of around 0.2 Ω/□ under wet/dry and stretched/unstretched conditions, while PVA films without prior treatment double in sheet resistance upon wetting or stretching the substrate. This low resistance of printed lines on salt-treated films can be preserved under multiple bending cycles of 0-90° and stretching cycles of 0-6% strain if the polymer is prestretched prior to inkjet printing.

Rotation Grids for Improved Electrical Properties of Inkjet-Printed Strain Gauges.

We report an image data driven approach for inkjet printing (IJP) to improve the electrical properties of printed metallic strain gauges (SGs). The examined SGs contain narrow conducting paths of multiple orientations and therefore suffer from two challenges: 1. The printing direction of inkjet printed conducting paths has an impact on film formation and electrical properties. 2. A loss-free rotation algorithm for IJP image data is lacking. New ways of IJP image data processing are required to compensate for quality-reducing effects. Novel grid types in terms of loss-free rotation algorithms are introduced. For this purpose, a new grid (e.g., 45° tilted) with a different grid constant is placed over a given pixel grid in such a way that all cell centers of the given pixel grid can be transferred to the rotated grid. Via straightening the tilt, the image data is rotated without interpolation and information loss. By applying these methods to measurement gratings of a full bridge with two perpendicular grating orientations, the influence on the manufacturing quality is investigated. It turns out that the electrical detuning of full bridges can be reduced by one order of magnitude compared to state-of-the-art printing by using so-called diagonal rotation grids.

Printed Potentiometric Nitrate Sensors for Use in Soil.

Plant-available nitrogen, often in the form of nitrate, is an essential nutrient for plant growth. However, excessive nitrate in the environment and watershed has harmful impacts on natural ecosystems and consequently human health. A distributed network of nitrate sensors could help to quantify and monitor nitrogen in agriculture and the environment. Here, we have developed fully printed potentiometric nitrate sensors and characterized their sensitivity and selectivity to nitrate. Each sensor comprises an ion-selective electrode and a reference electrode that are functionalized with polymeric membranes. The sensitivity of the printed ion-selective electrodes was characterized by measuring their potential with respect to a commercial silver/silver chloride reference electrode in varying concentrations of nitrate solutions. The sensitivity of the printed reference electrodes to nitrate was minimized with a membrane containing polyvinyl butyral (PVB), sodium chloride, and sodium nitrate. Selectivity studies with sulphate, chloride, phosphate, nitrite, ammonium, calcium, potassium, and magnesium showed that high concentrations of calcium can influence sensor behavior. The printed ion-selective and reference electrodes were combined to form a fully printed sensor with sensitivity of -48.0 ± 3.3 mV/dec between 0.62 and 6200 ppm nitrate in solution and -47 ± 4.1 mV/dec in peat soil.

3D Printing Silk-Based Bioresorbable Piezoelectric Self-Adhesive Holey Structures for In Vivo Monitoring on Soft Tissues.

Flexible and biocompatible adhesives with sensing capabilities can be integrated onto human body and organ surfaces, characterized by complex geometries, thus having the potential to sense their physiological stimuli offering monitoring and diagnosis of a wide spectrum of diseases. The challenges in this innovative field are the following: (i) the coupling method between the smart adhesive and the soft human substrates, (ii) the bioresorbable behavior of the material, and (iii) the electrical exchange with the substrate. Here, we introduce a multifunctional composite by mixing silk fibroin, featuring piezoelectric properties, with a soluble plant-derived polyphenol (i.e., chestnut tannin) modified with graphene nanoplatelets. This material behaves as a glue on different substrates and gives rise to high elongation at break, conformability, and adhesive performances to gastrointestinal tissues in a rat model and favors the printability via extrusion-based 3D printing. Exploiting these properties, we designed a bioresorbable 3D printed flexible and self-adhesive piezoelectric device that senses the motility once applied onto a phantom intestine and the hand gesture by signal translation. Experimental results also include the biocompatibility study using gastrointestinal cells. These findings could have applicability in animal model studies, and, thanks to the bioresorbable behavior of the materials, such an adhesive device could be used for monitoring the motility of the gastrointestinal tract and for the diagnosis of motility disorders.

Flow separation sensing on airfoil using a 3D printed biomimetic artificial hair sensor.

Small-scale unmanned air vehicles require lightweight, compact, and low-power sensors that encompass a variety of sensing modalities to enable flight control and navigation in challenging environments. Flow sensing is one such modality that has attracted much interest in recent years. In this paper, a micro-scale artificial hair sensor is developed to resolve both the direction and magnitude of airflow. The sensor structure employs a high-aspect ratio hair structure and a thin flexible membrane to facilitate the transduction of directional airflow to membrane deflection. The sensor readout is based on capacitive sensing and two pairs of electrodes orthogonal to each other are used to obtain airflow directional information. The sensor structure was fabricated using two-photon polymerization and integration onto a miniature printed circuit board to enable simple measurement. The sensor's responses to static displacement loading from different directions were characterized. The experimental results are in good agreement with the simulation results. Furthermore, the sensor's capability to measure the direction and magnitude of flow was demonstrated. Finally, the sensor was mounted on an airfoil and its ability to detect flow separation was verified.

Printed Low-Cost PEDOT:PSS/PVA Polymer Composite for Radiation Sterilization Monitoring.

During the γ-radiation sterilization process, the levels of radiation exposure to a medical device must be carefully monitored to achieve the required sterilization without causing deleterious effects on its intended physical and chemical properties. To address this issue, here we have demonstrated the development of an all-printed disposable low-cost sensor that exploits the change in electrical impedance of a semi-interpenetrating polymer network (SIPN) composed of poly(vinyl alcohol) (PVA) and poly(3,4-ethylenedioxythiophene):polystyrenesulfonate (PEDOT:PSS) as a functional polymer composite for radiation sterilization monitoring applications. Specifically, the PEDOT:PSS acts as the electrically conductive medium, while the PVA provides the ductility and stability of the printed sensors. During irradiation exposure, chain scission and cross-linking events occur concurrently in the PEDOT:PSS and PVA polymer chains, respectively. The concurrent scissoring of the PEDOT polymer and cross-linking of the PVA polymer network leads to the formation of a stable SIPN with reduced electrical conductivity, which was verified through FTIR, Raman, and TGA analysis. Systematic studies of different ratios of PEDOT:PSS and PVA mixtures were tested to identify the optimal ratio that provided the highest radiation sensitivity and stability performance. The results showed that PEDOT:PSS/PVA composites with 10 wt % PVA produced sensors with relative impedance changes of 30% after 25 kGy and up to 370% after 53 kGy (which are two of the most commonly used radiation exposure levels for sterilization applications). This composition showed high electrical impedance stability with less than ±5% change over 18 days after irradiation exposure. These findings demonstrate the feasibility of utilizing a printing technology for scalable manufacturing of low-cost, flexible radiation sensors for more effective monitoring of radiation sterilization processes.

Influence of filament aging and conductive additive in 3D printed sensors.

3D printing technology combined with electrochemical techniques have allowed the development of versatile and low-cost devices. However, some aspects need to be considered for the good quality and useful life of the sensors. In this work, we have demonstrated herein that the filament aging, the conductive material, and the activation processes (post-treatments) can influence the surface characteristics and the electrochemical performance of the 3D printed sensors. Commercial filaments and 3D printed sensors were morphologically, thermally, and electrochemically analyzed. The activated graphene-based (Black Magic®) sensor showed the best electrochemical response, compared to the carbon black-filament (Proto-Pasta®). In addition, we have proven that filament aging harms the performance of the sensors since the electrodes produced with three years old filament had a considerably lower intra-days reproducibility. Finally, the activated graphene-based sensor has shown the best performance for the electrochemical detection of bisphenol A, demonstrating the importance of evaluating and control the characteristics and quality of filaments to improve the mechanical, conductive, and electrochemical performance of 3D printed sensors.

A plug, print & play inkjet printing and impedance-based biosensing technology operating through a smartphone for clinical diagnostics.

Simplicity is one of the key feature for the spread of any successful technological product. Here, a method for rapid and low-cost fabrication of electrochemical biosensors is presented. This "plug, print & play" method involves inkjet-printing even in an office-like environment, without the need of highly specialized expertise or equipment, guaranteeing an ultra-fast idea to (scaled) prototype production time. The printed biosensors can be connected to a smartphone through its audio input for their impedance readout, demonstrating the validity of the system for point-of-care biosensing. Proper electrodes layout guarantees high sensitivity and is validated by finite element simulations. The introduction of a passivation method (wax printing) allowed to complete the devices fabrication process, increasing their sensitivity. Indeed, the wax allowed reducing the interference related to the parasitic currents flowing through the permeable coating of the employed substrates, which was used for the chemical sintering, thus avoiding the common thermal treatment after printing. As a case study, we used the devices to develop an electrochemical aptamer-based sensor for the rapid detection of neutrophil gelatinase-associated lipocalin (NGAL) in urine - a clinically important marker of acute kidney injury. The aptasensor platform is capable of detecting clinically relevant concentrations of NGAL with a simple and rapid smartphone readout. The developed technology may be extended in the future to continuous monitoring, taking advantage of its flexibility to integrate it in tubes, or to other diagnostic applications where cost/efficiency and rapidity of the research, development and implementation of point of care devices is a must.

Cavitas electrochemical sensors for the direct determination of salivary thiocyanate levels.

Noninvasive diagnosis using salivary samples to detect thiocyanate provides vital information on individual health. This article demonstrates the first example of a wearable sensing device to noninvasively assess thiocyanate levels. The customized screen-printed electrode system is integrated into a form of a mouthguard squarewave-voltammetric sensor toward the convenient and fast detection of the salivary biomarker within 15 s. The sensor with a protective film to mitigate the effect of biofouling offers high sensitivity and selectivity toward the detection of thiocyanate ions. Partial least square regression is applied to analyze the high-order squarewave-voltammetric data over the applied potential range of 0-1.75 V vs Ag/AgCl and quantify the thiocyanate concentration in a complex matrix. The mouthguard sensor operating under physiological conditions can monitor a wide range of thiocyanate (up to 11 mM) with a low detection limit of 30 µM. The demonstration introduces a unique approach, that obviates the requirement for blood sampling, to study thiocyanate levels of healthy people, cigarette smokers, or people with other health conditions. It is envisioned that the new cavitas device possesses a substantial promise for diverse biomedical diagnosis applications.

An Ascorbate Bluetooth© Analyzer for Quality Control of Fresh-Cut Parsley Supply Chain.

This work provides companies in the fresh-cut produce sector with an Ascorbate Bluetooth© Analyzer (ABA), a screen-printed sensor-based device for ascorbic acid (AA) detection, for quality control all along the supply chain. The amperometric detection of AA on fresh and fresh-cut parsley, under correct and incorrect storage temperature, allowed us to investigate the kinetics of AA decay in response to oxidative stress. The role of ascorbate oxidase (AOx) and ascorbate peroxidase (APx) was studied. ABA was used in situ by unskilled personnel. Treatments influenced AA decay kinetics, which were linear in fresh parsley, and non-linear in fresh-cut. Two hours at 28 °C immediately after chopping, the resilience of the fresh-cut parsley was reduced, even though the cold chain was restored. Two hours at -2 °C caused a rapid loss of AA until its complete decay after 72 h. Significant differences between treatments were observed in both the expression and activity of AOx and APx. ABA registered sudden changes of parsley AA following unpredicted variations of temperature during processing or transport. It was useful to remedy the effects of unexpected flaws in the cold chain, which can be proposed for quality preservation of different fresh-cut produce.

Evaluation of Inkjet-Printed Reduced and Functionalized Water-Dispersible Graphene Oxide and Graphene on Polymer Substrate-Application to Printed Temperature Sensors.

The present work reports on the detailed electro-thermal evaluation of a highly water dispersible, functionalized reduced graphene oxide (f-rGO) using inkjet printing technology. Aiming in the development of printed electronic devices, a flexible polyimide substrate was used for the structures' formation. A direct comparison between the f-rGO ink dispersion and a commercial graphene inkjet ink is also presented. Extensive droplet formation analysis was performed in order to evaluate the repeatable and reliable jetting from an inkjet printer under study. Electrical characterization was conducted and the electrical characteristics were assessed under different temperatures, showing that the water dispersion of the f-rGO is an excellent candidate for application in printed thermal sensors and microheaters. It was observed that the proposed f-rGO ink presents a tenfold increased temperature coefficient of resistance compared to the commercial graphene ink (G). A successful direct interconnection implementation of both materials with commercial Ag-nanoparticle ink lines was also demonstrated, thus allowing the efficient electrical interfacing of the printed structures. The investigated ink can be complementary utilized for developing fully printed devices with various characteristics, all on flexible substrates with cost-effective, few-step processes.

Modelling of Anisotropic Electrical Conduction in Layered Structures 3D-Printed with Fused Deposition Modelling.

3D-printing conductive structures have recently been receiving increased attention, especially in the field of 3D-printed sensors. However, the printing processes introduce anisotropic electrical properties due to the infill and bonding conditions. Insights into the electrical conduction that results from the anisotropic electrical properties are currently limited. Therefore, this research focuses on analytically modeling the electrical conduction. The electrical properties are described as an electrical network with bulk and contact properties in and between neighbouring printed track elements or traxels. The model studies both meandering and open-ended traxels through the application of the corresponding boundary conditions. The model equations are solved as an eigenvalue problem, yielding the voltage, current density, and power dissipation density for every position in every traxel. A simplified analytical example and Finite Element Method simulations verify the model, which depict good correspondence. The main errors found are due to the limitations of the model with regards to 2D-conduction in traxels and neglecting the resistance of meandering ends. Three dimensionless numbers are introduced for the verification and analysis: the anisotropy ratio, the aspect ratio, and the number of traxels. Conductive behavior between completely isotropic and completely anisotropic can be modeled, depending on the dimensionless properties. Furthermore, this model can be used to explain the properties of certain 3D-printed sensor structures, like constriction-resistive strain sensors.