We propose a new facile electrochemical sensing platform for determination of urea, based on a glassy carbon electrode (GCE) modified with nickel cobalt oxide (NiCo 2 O 4 ) nanoneedles. These nanoneedles are used for the first time for highly sensitive determination of urea with the lowest detection limit (1 μM) ever reported for the non-enzymatic approach. The nanoneedles were grown through a simple and low-temperature aqueous chemical method. We characterized the structural and morphological properties of the NiCo 2 O 4 nanoneedles by TEM, SEM, XPS and XRD. The bimetallic nickel cobalt oxide exhibits nanoneedle morphology, which results from the self-assembly of nanoparticles. The NiCo 2 O 4 nanoneedles are exclusively composed of Ni, Co, and O and exhibit a cubic crystalline phase. Cyclic voltammetry was used to study the enhanced electrochemical properties of a NiCo 2 O 4 nanoneedle-modified GCE by overcoming the typical poor conductivity of bare NiO and Co 3 O 4 . The GCE-modified electrode is highly sensitive towards urea, with a linear response (R 2 = 0.99) over the concentration range 0.01-5 mM and with a detection limit of 1.0 μM. The proposed non-enzymatic urea sensor is highly selective even in the presence of common interferents such as glucose, uric acid, and ascorbic acid. This new urea sensor has good viability for urea analysis in urine samples and can represent a significant advancement in the field, owing to the simple and cost-effective fabrication of electrodes, which can be used as a promising analytical tool for urea estimation.

Manufacturing of electronic devices via printing techniques is often considered to be an environmentally friendly approach, partially due to the efficient utilization of materials. Traditionally, printed electronic components (e.g., sensors, transistors, and displays) are relying on flexible substrates based on plastic materials; this is especially true in electronic display applications where, most of the times, a transparent carrier is required in order to enable presentation of the display content. However, plastic-based substrates are often ruled out in end user scenarios striving toward sustainability. Paper substrates based on ordinary cellulose fibers can potentially replace plastic substrates, but the opaqueness limits the range of applications where they can be used. Herein, electrochromic displays that are manufactured, via screen printing, directly on state-of-the-art fully transparent substrates based on nanocellulose are presented. Several different nanocellulose-based substrates, based on either nanofibrillated or nanocrystalline cellulose, are manufactured and evaluated as substrates for the manufacturing of electrochromic displays, and the optical and electrical switching performances of the resulting display devices are reported and compared. The reported devices do not require the use of metals and/or transparent conductive oxides, thereby providing a sustainable all-printed electrochromic display technology.

Fast and accurate detection of microorganisms is of key importance in clinical analysis and in food and water quality monitoring. Salmonella typhimurium is responsible for about a third of all cases of foodborne diseases and consequently, its fast detection is of great importance for ensuring the safety of foodstuffs.We report the development of a label-free impedimetric aptamer-based biosensor for S. typhimurium detection. The aptamer biosensor was fabricated by grafting a diazonium-supporting layer onto screen-printed carbon electrodes (SPEs), via electrochemical or chemical approaches, followed by chemical immobilisation of aminated-aptamer. FTIR-ATR, contact angle and electrochemical measurements were used to monitor the fabrication process. Results showed that electrochemical immobilisation of the diazonium-grafting layer allowed the formation of a denser aptamer layer, which resulted in higher sensitivity. The developed aptamer-biosensor responded linearly, on a logarithm scale, over the concentration range 1×101 to 1×108 CFU mL-1, with a limit of quantification (LOQ) of 1×101 CFU mL-1 and a limit of detection (LOD) of 6 CFU mL-1. Selectivity studies showed that the aptamer biosensor could discriminate S. typhimurium from 6 other model bacteria strains. Finally, recovery studies demonstrated its suitability for the detection of S. typhimurium in spiked (1×102, 1×104 and 1×106 CFU mL-1) apple juice samples.

Mobile diagnostics for healthcare, food safety and environmental monitoring, demand a new generation of inexpensive sensing systems suitable for production in high volume. Herein we report on the development of a new disposable electrochemical instrument exploiting the latest advances in printed electronics and printed biosensors. The current system is manufactured under ambient conditions with all interconnections printed; electrochemical measurements and data elaboration are realized by the integration onto the platform of two chips: a MICROCHIP-PIC24F16KA101 and a Texas Instrument's LMP91000. A PEDOT.PSS vertical electrochromic display (VECD) is also incorporated into the system to visualize the data. A printed Enfucell 3V manganese dioxide battery was used to deliver the required power. Finally, in order to demonstrate the utility of the system, screen-printed sensors for the detection of glucose were added and the performance of the overall system was evaluated.

The quantification of urea is of the utmost importance not only in medical diagnosis, where it serves as a potential indicator of kidney and liver disfunction, but also in food safety and environmental control. Here, we describe a urea biosensor based on urease entrapped in a crosslinked gelatin hydrogel, deposited onto a fully printed PEDOT:PSS-based organic electrochemical transistor (OECT). The device response is based on the modulation of the channel conductivity by the ionic species produced upon urea hydrolysis catalyzed by the entrapped urease. The biosensor shows excellent reproducibility, a limit of detection as low as 1 μM and a response time of a few minutes. The fabrication of the OECTs by screen-printing on flexible substrates ensures a significant reduction in manufacturing time and costs. The low dimensionality and operational voltages (0.5 V or below) of these devices contribute to make these enzymatic OECT-based biosensors as appealing candidates for high-throughput monitoring of urea levels at the point-of-care or in the field.

Stretchable organic electrochemical transistors (OECTs) are promising for wearable applications within biosensing, bio-signal recording, and addressing circuitry. Efficient large-scale fabrication of OECTs can be performed with printing methods but to date there are no reports on high-performance fully printed stretchable OECTs. Herein, this challenge is addressed by developing fully screen-printed stretchable OECTs based on an architecture that minimizes electrochemical side reactions and improves long-term stability. Fabrication of the OECTs is enabled by in-house development of three stretchable functional screen-printing inks and related printing processes. The stretchable OECTs show good characteristics in terms of transfer curves, output characteristics, and transient response up to 100% static strain and 500 strain cycles at 25% and 50% strain. The strain insensitivity of the OECTs can be further improved by strain conditioning, resulting in stable performance up to 50% strain. Finally, an electrochromic smart pixel is demonstrated by connecting a stretchable OECT to a stretchable electrochromic display. It is believed that the development of screen-printed stretchable electrochemical devices, and OECTs in particular, will pave the way for their use in wearable applications and commercial products. © 2023 The Authors. 

High-throughput production methods such as screen printing can bring stretchable electronics out of the lab into the market. Most stretchable conductor inks for screen printing are based on silver nanoparticles or flakes due to their favorable performance-to-cost ratio, but silver is prone to tarnishing and corrosion, thereby limiting the stability of such conductors. Here, we report on a cost-efficient and scalable approach to resolve this issue by developing screen printable inks based on silver flakes chemically coated by a thin layer of gold. The printed stretchable AgAu conductors reach a conductivity of 8500 S cm-1, remain conductive up to 250% strain, show excellent corrosion and tarnishing stability, and are used to demonstrate wearable LED and NFC circuits. The reported approach is attractive for smart clothing, as the long-term functionality of such devices is expected in a variety of environments. © 2023 The Authors.

Conventional electronics have been highlighted as a very unsustainable technology; hazardous wastes are produced both during their manufacturing but also, due to their limited recyclability, during their end of life cycle (e.g. disposal in landfill). In recent years additive manufacturing processes (i.e. screen printing) have attracted significant interest as a more sustainable approach to electronic manufacturing (printed electronics). Despite the field of printed electronics addressing some of the issues related to the manufacturing of electronics, many components and inks are still considered hazardous to the environment and are difficult to recycle. Here we present the development of a low environmental impact carbon ink based on a non-hazardous solvent and a cellulosic matrix (nanocellulose) and its implementation in electrochromic displays (ECDs) and supercapacitors. As part of the reported work, a different protocol for mixing carbon and cellulose nanofibrils (rotation mixing and high shear force mixing), nanocellulose of different grades and different carbon: nanocellulose ratios were investigated and optimized. The rheology profiles of the different inks showed good shear thinning properties, demonstrating their suitability for screen-printing technology. The printability of the developed inks was excellent and in line with those of reference commercial carbon inks. Despite the lower electrical conductivity (400 S m-1 for the developed carbon ink compared to 1000 S m-1 for the commercial inks), which may be explained by their difference in composition (carbon content, density and carbon derived nature) compared to the commercial carbon, the developed ink functioned adequately as the counter electrode in all screen-printed ECDs and even allowed for improved supercapacitors compared to those utilizing commercial carbon inks. In this sense, the supercapacitors incorporating the developed carbon ink in the current collector layer had an average capacitance = 97.4 mF cm-2 compared to the commercial carbon ink average capacitance = 61.6 mF cm-2. The ink development reported herein provides a step towards more sustainable printed green electronics. © 2021 The Author(s).

Biological systems use a large variety of ions and molecules of different sizes for signaling. Precise electronic regulation of biological systems therefore requires an interface which translates the electronic signals into chemically specific biological signals. One technology for this purpose that has been developed during the last decade is the organic electronic ion pump (OEIP). To date, OEIPs have been fabricated by micropatterning and labor-intensive manual techniques, hindering the potential application areas of this promising technology. Here we show, for the first time, fully screen-printed OEIPs. We demonstrate a large-area printed design with manufacturing yield >90%. Screen-printed cation- and anion-exchange membranes are both demonstrated with promising ion selectivity and performance, with transport verified for both small ions (Na⁺, K⁺, Cl^–) and biologically-relevant molecules (the cationic neurotransmitter acetylcholine, and the anionic anti-inflammatory salicylic acid). These advances open the 'iontronics' toolbox to the world of printed electronics, paving the way for a broader arena for applications.

The development of electronics with net zero carbon emissions through more efficient and environmentally friendly materials and processes is still a challenge. Here, alternative chemical synthesis routes of metal conductive nanoparticles, based on biodegradable materials are explored, such as nickel, iron–nickel alloy and iron nanoparticles, to be used, in the long term, as fillers in inks for inject printing. Thus, Ni and FeNi metal nanoparticles of 25–12 nm, forming aggregates of 614–574 nm, respectively, are synthesized in water in the presence of a polyol and a reducing agent and under microwave heating that enables a more uniform and fast heating. Iron nanoparticles of 120 ± 40 nm are synthesized in polyol that limits the aggregation and the oxidation degree. Commercial metal nanoparticles of iron and nickel, are coated with ethylene glycol and used for comparison. The conductivity of nanoparticles when pressed into pellets remains similar for both commercial and synthesized samples. However, when deposited on a strip line and heated, synthesized Ni, FeNi, and Fe nanoparticles show significant conductivity and interesting magnetic properties. It is demonstrated that the nanosize facilitates sintering at reduced temperatures and the capping agents prevent oxidation, resulting in promising conductive fillers for printed electronic applications. 

Redox labeled DNAs are of increasing interest for the fabrication of next generation molecular tools. In the present work we are investigating the use of various redox labeled dNTPs, ddNTPs and DNA primers for use in detection of diseases. We have reported the use of Polyoxometalate (POM) labeled DNA primers and dNTPs for use in PCR and subsequently used for direct electrochemical detection of PCR products. The use of POM labeled DNAs in PCR enabled us to check the compatibility with polymerases and PCR incorporability of the modified DNAs. Furthermore we have investigated the solid-phase array based primer extension (é-PEX) with redox labelled ddNTPs (ferrocene (Fc), anthraquinone (AQ) phenothiazine (PTZ) and methylene blue (MB)) to prove the strategy of detection of single nucleotide polymorphisms using the labeled ddNTPs. This strategy will allow the development of cost-effective, rapid and user-friendly platform for the screening of known and unknown genetic mutations.

The photochemical core of every photosynthetic apparatus is the reaction center, a transmembrane enzyme that converts photons into charge-separated states across the biological membrane with an almost unitary quantum yield. A light-responsive organic transistor architecture, which converts light into electrical current by exploiting the efficiency of this biological machinery, is presented. Proper surface tailoring enables the integration of the bacterial reaction center as photoactive element in organic transistors, allowing the transduction of its photogenerated voltage into photomodulation of the output current up to two orders of magnitude. This device architecture, termed light-responsive electrolyte-gated organic transistor, is the prototype of a new generation of low-power hybrid bio-optoelectronic organic devices.

The transition to a sustainable society is driving the development of green electronic solutions designed to have a minimal environmental impact. One promising route to achieve this goal is to construct electronics from biobased materials like cellulose, which is carbon neutral, non‐toxic, and recyclable. This is especially true for internet‐of‐things devices, which are rapidly growing in number and are becoming embedded in every aspect of our lives. Here, paper‐based sensor circuits are demonstrated, which use triboelectric pressure sensors to help elderly people communicate with the digital world using an interface in the form of an electronic “book”, which is more intuitive to them. The sensors are manufactured by screen printing onto flexible paper substrates, using in‐house developed cellulose‐based inks with non‐hazardous solvents. The triboelectric sensor signal, generated by the contact between a finger and chemically modified cellulose, can reach several volts, which can be registered by a portable microcontroller card and transmitted by Bluetooth to any device with an internet connection. Apart from the microcontroller (which can be easily removed), the whole system can be recycled at the end of life. A triboelectric touch interface, manufactured using printed electronics on flexible paper substrates, using cellulose‐based functional inks is demonstrated. These metal‐free green electronics circuits are implemented in an “electronic book” demonstrator, equipped with wireless communication that can control remote devices, as a step toward sustainable and recyclable internet‐of‐things devices.

Triboelectric nanogenerators (TENGs) are a new class of energy harvesting devices that have the potential to become a dominating technology for producing renewable energy. The versatility of their designs allows TENGs to harvest mechanical energy from sources like wind and water. Currently used renewable energy technologies have a restricted number of materials from which they can be constructed, such as metals, plastics, semiconductors, and rare-earth metals. These materials are all non-renewable in themselves as they require mining/drilling and are difficult to recycle at end of life. TENGs on the other hand can be built from a large repertoire of materials, including materials from bio-based sources. Here, a TENG constructed fully from wood-derived materials like lignin, cellulose, paper, and cardboard, thus making it 100% green, recyclable, and even biodegradable, is demonstrated. The device can produce a maximum voltage, current, and power of 232 V, 17 mA m–2, and 1.6 W m–2, respectively, which is enough to power electronic systems and charge 6.5 µF capacitors. Finally, the device is used in a smart package application as a self-powered impact sensor. The work shows the feasibility of producing renewable energy technologies that are sustainable both with respect to their energy sources and their material composition. © 2022 The Authors. 

Paper electronics is a viable alternative to traditional electronics, leading to more sustainable electronics. Many challenges still require solutions before paper electronics become mainstream. Here, we present a solution to enable the manufacturing of reflective all-printed organic electrochromic displays (OECDs) on paper substrates; devices that are usually printed on transparent substrates, for example, plastics. In order to operate on opaque paper substrates, an architecture for reversely printed OECDs (rOECDs) is developed. In this architecture, the electrochromic layer is printed as the last functional layer and can therefore be viewed from the print side. Square shaped 1 cm2 rOECDs are successfully screen printed on paper, with a high manufacturing yield exceeding 99%, switching times <3 s and high color contrast (ΔE* > 27). Approximately 60% of the color is retained after 15 min in open-circuit mode. Compared to the conventional screen printed OECD architectures, the rOECDs recover approximately three times faster from storage in a dry environment, which is particularly important in systems where storage in low humidity atmosphere is required, for example, in many biosensing applications. Finally, a more complex rOECD with 9 individually addressable segments is successfully screen printed and demonstrated.

Low-cost, minimally invasive sensors able to provide real-time monitoring of wound infection can enable the optimization of healthcare resources in chronic wounds management. Here, a novel printed organic electrochemical transistors (OECT) biosensor for monitoring uric acid (UA), a bacterial infection biomarker in wounds, is demonstrated in artificial wound exudate. The sensor exploits the enzymatic conversion of UA to 5-hydroxyisourate, catalyzed by Uricase entrapped in a dual-ionic-layer hydrogel membrane casted onto the gate. The sensor response is based on the catalytic oxidation of the hydrogen peroxide, generated as part of the Uricase regeneration process, at the Pt modified gate. The proposed dual membrane avoids the occurrence of nonspecific faradic reactions as, for example, the direct oxidation of UA or other electroactive molecules that would introduce a potentially false negative response. The biosensor is robust and its response is reproducible both in phosphate buffer saline and in complex solutions mimicking the wound exudate. The sensor has a high sensitivity in the range encompassing the pathological levels of UA in wounds (<200 μm) exhibiting a limit of detection of 4.5 μm in artificial wound exudate. All these characteristics make this OECT-based biosensor attractive for wound monitoring interfaced to the patient.

Biosensors can deliver the rapid bacterial detection that is needed in many fields including food safety, clinical diagnostics, biosafety and biosecurity. Whole-cell imprinted polymers have the potential to be applied as recognition elements in biosensors for selective bacterial detection. In this paper, we report on the use of 3-aminophenylboronic acid (3-APBA) for the electrochemical fabrication of a cell-imprinted polymer (CIP). The use of a monomer bearing a boronic acid group, with its ability to specifically interact with cis-diol, allowed the formation of a polymeric network presenting both morphological and chemical recognition abilities. A particularly beneficial feature of the proposed approach is the reversibility of the cis-diol-boronic group complex, which facilitates easy release of the captured bacterial cells and subsequent regeneration of the CIP. Staphylococcus epidermidis was used as the model target bacteria for the CIP and electrochemical impedance spectroscopy (EIS) was explored for the label-free detection of the target bacteria. The modified electrodes showed a linear response over the range of 103–107 cfu/mL. A selectivity study also showed that the CIP could discriminate its target from non-target bacteria having similar shape. The CIPs had high affinity and specificity for bacterial detection and provided a switchable interface for easy removal of bacterial cell.

Here we demonstrate the use of a functional dopant as a fast and simple way to tune the chemical affinity and selectivity of polypyrrole films. More specifically, a boronic-functionalised dopant, 4-N-Pentylphenylboronic Acid (PBA), was used to provide to polypyrrole films with enhanced affinity towards diols. In order to prove the proposed concept, two model systems were explored: (i) the capture and the electrochemical detection of dopamine and (ii) the adhesion of bacteria onto surfaces. The chemisensor, based on overoxidised polypyrrole boronic doped film, was shown to have the ability to capture and retain dopamine, thus improving its detection; furthermore the chemisensor showed better sensitivity in comparison with overoxidised perchlorate doped films. The adhesion of bacteria, Deinococcus proteolyticus, Escherichia coli, Streptococcus pneumoniae and Klebsiella pneumoniae, onto the boric doped polypyrrole film was also tested. The presence of the boronic group in the polypyrrole film was shown to favour the adhesion of sugar-rich bacterial cells when compared with a control film (Dodecyl benzenesulfonate (DBS) doped film) with similar morphological and physical properties. The presented single step synthesis approach is simple and fast, does not require the development and synthesis of functional monomers, and can be easily expanded to the electrochemical, and possibly chemical, fabrication of novel functional surfaces and interfaces with inherent pre-defined sensing and chemical properties.

In this paper, we present a non-fluidic microsystem for the simultaneous visualization and electrochemical evaluation of confined, growing bacteria on solid media. Using a completely automated platform, real-time monitoring of bacterial and image-based computer characterization of growth were performed. Electrochemical tests, using Escherichia coli K-12 as the model microorganism, revealed the development of a faradaic process at the bacteria-microelectrode interface inside the microsystem, as implied by cyclic voltammetry and electrochemical impedance spectrometry measurements. The electrochemical information was used to determine the moment in which bacteria colonized the electrode-enabled area of the microsystem. This microsystem shows potential advantages for long-term electrochemical monitoring of the extracellular environment of cell culture and has been designed using readily available technologies that can be easily integrated in routine protocols. Complementarily, these methods can help elucidate fundamental questions of the electron transfer of bacterial cultures and are potentially feasible to be integrated into current characterization techniques.

The society is transitioning towards a circular economy and the Digital Cellulose Center (DCC) that develops green electronics may play an important role in it. The research within the DCC focuses on the topic of digital cellulose, where cellulose is combined with electroactive material, making it possible to develop electrically active cellulose products that can communicate with the digital world while remaining sustainable. This could mean entirely new types of active packaging solutions, able to sense and adapt to their surroundings, or paper rolls able to store energy from solar cells or wind power [1]. This document offers guidance for the DCC stakeholders on the choice of sustainable materials for green electronics, focusing on the two life cycle phases of a product: • Raw materials • End-of-life Since the DCC green electronics are still in the development stage, a future scenario analysis has been applied in order to envision the possible future outcomes. The DCC green electronics have been explored in two opposite future scenarios: • Stuck in the Mud – A business-as-usual scenario, where the year 2045 is more or less the same as year 2022. • Circular Dawn – Where the circular economy has become a new normal and the whole society is thriving in a resource-efficient, circular and biobased economy. The guideline contains a sustainability checklist adapted to the needs of the DCC stakeholders for more informed decision-making and for being able to drive the development towards a circular economy, i. e. the future scenario Circular Dawn.

The advent of the Internet of Things and the growing interest in continuous monitoring by wearables have created a need for conformable and stretchable displays. Electrochromic displays (ECDs) are receiving attention as a cost-effective solution for many simple applications. However, stretchable ECDs have yet to be produced in a robust, large scale and cost-efficient manner. Here we develop a process for making fully screen printed stretchable ECDs. By evaluating commercially available inks with respect to electromechanical properties, including electrochromic PEDOT:PSS inks, our process can be directly applied in the manufacturing of stretchable organic electronic devices. The manufactured ECDs retained colour contrast with useful switching times at static strains up to 50% and strain cycling up to 30% strain. To further demonstrate the applicability of the technology, double-digit 7-segment ECDs were produced, which could conform to curved surfaces and be mounted onto stretchable fabrics while remaining fully functional. Based on their simplicity, robustness and processability, we believe that low cost printed stretchable ECDs can be easily scaled up and will find many applications within the rapidly growing markets of wearable electronics and the Internet of Things. © 2021 The Author(s). 

This study illustrates an innovative way to fabricate inkjet-printed tracks by sequential printing of Zn nanoparticle ink and curing ink for low temperature in situ chemical sintering. Employing chemical curing in place of standard sintering methods leads to the advantages of using flexible substrates that may not withstand the high thermal budgets of the standard methods. A general formulation engineering method is adopted to produce highly concentrated Zn ink which is cured by inkjet printing an over-layer of aqueous acetic acid which is the curing agent. The experimental results reveal that a narrow window of acid concentration of curing ink plays a crucial role in determining the electrical properties of the printed Zn nanoparticles. Highly conductive (~105 S m−1) and mechanically flexible printed Zn features are achieved. In addition, from systematic material characterization, we obtain an understanding of the curing mechanism. Finally, a touch sensor circuit is demonstrated involving all-Zn printed conductive tracks. © 2021, The Author(s).

Microfluidic surface chemistry can enable control of capillary-driven flow without the need for bulky external instrumentation. A novel pondered nonhomogeneous coating defines regions with different wetting properties on the microchannel walls. It changes the curvature of the liquid–air meniscus at various channel cross-sections and consequently leads to different capillary pressures, which is favorable in the strive toward automatic flow control. This is accomplished by the deposition of hydrophilic coatings on the surface of multilevel 3D-printed (3DP) microfluidic devices via inkjet printing, thereby retaining the surface hydrophilicity for at least 6 months of storage. To the best of our knowledge, this is the first demonstration of capillary flow control in 3DP microfluidics enabled by inkjet printing. The method is used to create “stop” and “delay” valves to enable preprogrammed capillary flow for sequential release of fluids. To demonstrate further utilization in point-of-care sensing applications, screen printed organic electrochemical transistors are integrated within the microfluidic chips to sense, sequentially and independently from external actions, chloride anions in the (1–100) × 10−3 m range. The results present a cost-effective fabrication method of compact, yet comprehensive, all-printed sensing platforms that allow fast ion detection (<60 s), including the capability of automatic delivery of multiple test solutions. © 2023 The Authors. 

This work demonstrates sensitive and low-cost piezoelectric sensors on skin-friendly, ultrathin, and conformable substrates combined with organic electrochemical transistors (OECTs) for the detection and amplification of alternating low-voltage input signals. The fully screen-printed (SP) piezoelectric sensors were manufactured on commercially available tattoo paper substrates, while the all-printed OECTs, relying on an extended gate electrode architecture, were manufactured either by solely using SP or by combining SP and aerosol jet printing (AJP) on PET substrates. Applying a low-voltage signal (±25 mV) to the gate electrode of the SP+AJP OECT results in approximately five times higher current modulation as compared to the fully SP reference OECT. The tattoo paper-based substrate enables transfer of the SP piezoelectric sensor to the skin, which in turn allows for radial pulse monitoring when combined with the SP+AJP OECT; this is possible due to the ability of the conformable sensor to convert mechanical vibrations into voltage signals along with the highly sensitive current modulation ability of the transistor device to further amplify the output signal. The results reported herein pave the way toward all-printed fully conformable wearable devices with high sensitivity to be further utilized for the real-time monitoring of electrophysiological signals.

Abstract This study reports on the first all-printed vertically stacked organic electrochemical transistors (OECTs) operating in accumulation mode; the devices, relying on poly([4,4?-bis(2-(2-(2-methoxyethoxy)ethoxy)ethoxy)-2,2?-bithiophen-5,5?-diyl]-alt-[thieno[3,2-b]thiophene-2,5-diyl]) (pgBTTT) as the active channel material, are fabricated via a combination of screen and inkjet printing technologies. The resulting OECTs (W/L ≈5) demonstrate good switching performance; gm, norm ≈13 mS cm?1, µC* ≈21 F cm?1 V?1 s?1, ON?OFF ratio > 104 and good cycling stability upon continuous operation for 2 h. The inkjet printing process of pgBTTT is established by first solubilizing the polymer in dihydrolevoglucosenone (Cyrene), a non-toxic, cellulose-derived, and biodegradable solvent. The resulting ink formulations exhibit good jettability, thereby providing reproducible and stable p-type accumulation mode all-printed OECTs with high performance. Besides the environmental and safety benefits of this solvent, this study also demonstrates the assessment of how the solvent affects the performance of spin-coated OECTs, which justifies the choice of Cyrene as an alternative to commonly used harmful solvents such as chloroform, also from a device perspective. Hence, this approach shows a new possibility of obtaining more sustainable printed electronic devices, which will eventually result in all-printed OECT-based logic circuits operating in complementary mode.

This work demonstrates a novel fabrication approach based on the combination of screen and aerosol jet printing to manufacture fully printed organic electrochemical transistors (OECTs) and OECT-based logic circuits on PET substrates with superior performances. The use of aerosol jet printing allows for a reduction of the channel width to ≈15 µm and the estimated volume by a factor of ≈40, compared to the fully screen printed OECTs. Hence, the OECT devices and OECT-based logic circuits fabricated with the proposed approach emerge with a high ON/OFF ratio (103–104) and remarkably fast switching response, reaching an ON/OFF ratio of &gt;103 in 4–8 ms, which is further demonstrated by a propagation delay time of just above 1 ms in OECT-based logic inverter circuits operated at a frequency of 100 Hz. All-printed monolithically integrated OECT-based five-stage ring oscillator circuits further validated the concept with a resulting self-oscillation frequency of 60 Hz. © 2022 The Authors.

The need for more sustainable printed electronics has emerged in the past years. Due to this, the use of nanocellulose (NC) extracted from cellulose has recently been demonstrated to provide interesting materials such as functional inks and transparent flexible films due to its properties. Its high specific surface area together with the high content of reactive hydroxyl groups provide a highly tailorable surface chemistry with applications in ink formulations as a stabilizing, capping, binding and templating agent. Moreover, NC mechanical, physical and thermal properties (high strength, low porosity and high thermal stability, respectively) provide an excellent alternative for the currently used plastic films. In this work, we present a process for the production of water-based conductive inks that uses NC both as a template for silver nanoparticles (Ag NPs) formation and as an ink additive for ink formulation. The new inks present an electrical conductivity up to 2 × 106 S/m, which is in the range of current commercially available conductive inks. Finally, the new Ag NP/NC-based conductive inks have been tested to fabricate NFC antennas by screen-printing onto NC-coated paper, demonstrating to be operative.

Hydrogels are of great importance for functionalizing sensors and microfluidics, and poly(ethylene glycol) dimethacrylate (PEG-DMA) is often used as a viscosifier for printable hydrogel precursor inks. In this study, 1–10 kDa PEG-DMA based hydrogels were characterized by gravimetric and electrochemical methods to investigate the diffusivity of small molecules and proteins. Swelling ratios (SRs) of 14.43–9.24, as well as mesh sizes ξ of 3.58–6.91 nm were calculated, and it was found that the SR correlates with the molar concentration of PEG-DMA in the ink (MCI) (SR = 0.1127 × MCI + 8.3256, R2 = 0.9692) and ξ correlates with the molecular weight (Mw) (ξ = 0.3382 × Mw + 3.638, R2 = 0.9451). To investigate the sensing properties, methylene blue (MB) and MB-conjugated proteins were measured on electrochemical sensors with and without hydrogel coating. It was found that on sensors with 10 kDa PEG-DMA hydrogel modification, the DPV peak currents were reduced to 92 % for MB, 73 % for MB-BSA, and 23 % for MB-IgG. To investigate the diffusion properties of MB(-conjugates) in hydrogels with 1–10 kDa PEG-DMA, diffusivity was calculated from the current equation. It was found that diffusivity increases with increasing ξ. Finally, the release of MB-BSA was detected after drying the MB-BSA-containing hydrogel, which is a promising result for the development of hydrogel-based reagent reservoirs for biosensing. 

Wood is an inherently hygroscopic material which tends to absorb moisture from its surrounding. Moisture in wood is a determining factor for the quality of wood being employed in construction, since it causes weakening, deformation, rotting, and ultimately leading to failure of the structures resulting in costs to the economy, the environment, and to the safety of residents. Therefore, monitoring moisture in wood during the construction phase and after construction is vital for the future of smart and sustainable buildings. Employing bio-based materials for the construction of electronics is one way to mitigate the environmental impact of such electronics. Herein, a bio-graphene sensor for monitoring the moisture inside and around wooden surfaces is fabricated using laser-induced graphitization of a lignin-based ink precursor. The bio-graphene sensors are used to measure humidity in the range of 10% up to 90% at 25 °C. Using laser induced graphitization, conductor resistivity of 18.6 Ω sq−1 is obtained for spruce wood and 57.1 Ω sq−1 for pine wood. The sensitivity of sensors fabricated on spruce and pine wood is 2.6 and 0.74 MΩ per % RH. Surface morphology and degree of graphitization are investigated using scanning electron microscopy, Raman spectroscopy, and thermogravimetric analysis methods. © 2023 The Authors. 

Energy harvesting from photosynthetic membranes, proteins, or bacteria through bio-photovoltaic or bio-electrochemical approaches has been proposed as a new route to clean energy. A major shortcoming of these and solar cell technologies is the underutilization of solar irradiation wavelengths in the IR region, especially those in the far IR region. Here, a biohybrid energy-harvesting device is demonstrated that exploits IR radiation, via convection and thermoelectric effects, to improve the resulting energy conversion performance. A composite of nanocellulose and the conducting polymer system poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) is used as the anode in biohybrid cells that includes thylakoid membranes (TMs) and redox mediators (RMs) in solution. By irradiating the conducting polymer electrode by an IR light-emitting diode, a sixfold enhancement in the harvested bio-photovoltaic power is achieved, without compromising stability of operation. Investigation of the output currents reveals that IR irradiation generates convective heat transfer in the electrolyte bulk, which enhances the redox reactions of RMs at the anode by suppressing diffusion limitations. In addition, a fast-transient thermoelectric component, originating from the PEDOT:PSS-nanocellulose-electrolyte interphase, further increases the bio-photocurrent. These results pave the way for the development of energy-harvesting biohybrids that make use of heat, via IR absorption, to enhance energy conversion efficiency. 

Porous carbon materials are common materials used for sensor and absorbent applications. A novel approach for functionalizing porous carbons through the impregnation of porous carbon black with benzoxazine monomers, followed by thermal polymerization is introduced herein. The method not only establishes a new avenue for the functionalization of porous carbons but also endows the resulting material with both copper ion-binding and sensing properties. We showcase the versatility of the technique by illustrating that the polymerization of phenols with benzoxazine monomers serves as an extra tool to customize absorption- and sensing properties. Experimental validation involved testing the method on carbon black as a porous substrate, which was impregnated with both bisphenol-a benzoxazine and a combination of bisphenol-a benzoxazine and alizarin. The resulting materials were assessed for their dual functionality as both an absorbent and a sensor for copper ions by varied copper ion concentrations and exposure times. The dye absorption test demonstrated a notable capacity to accumulate copper ions from dilute solutions. Electrochemical characterization further confirmed the effectiveness of the modified carbons, as electrodes produced from inks were successful in detecting copper ions accumulated from 50 μM Cu2+ solutions. With this work, we aspire to set the steppingstone towards a facile functionalization of porous carbon materials towards water purification applications. © 2024 The Authors

An ISM band sectorial compact antenna working at 868 MHz is presented in this paper. The antenna is designed to have very low perturbations in terms of radiation pattern, bandwidth and input impedance when mounted on different environments at the rear (i.e. wood, plastic or metal support). Furthermore, the PIFA topology of the antenna allows an easy matching either to a 50 Ohm input impedance for IoT/LoRA applications or to a complex impedance value for RFID applications with the help of a simple matching circuit. 

Organic electrochemical transistors (OECTs) operated in the faradic regime were shown as outperforming transducers of bioelectric signals in vitro and in vivo. Fabrication by additive manufacturing techniques fosters OECTs as ideal candidates for point-of-care applications, as well as imposes limitations on the choice of materials and their processing conditions. Here, we address the question of how the response of fully printed OECTs depends on gate electrode material. Toward this end, we investigate the redox processes underlying the operation of OECTs under faradic regime, to show OECTs with carbon gate (C-gate) that exhibit no current modulation gate voltages <1.2 V. This is a hallmark that no interference with the faradic operation of the device enabled by redox processes occurs when operating C-gate OECTs in the low-voltage range as label-free biosensors for the detection of electroactive (bio)molecules. To tune the faradic response of the device, we electrodeposited Au on the carbon gate (Au-C-gate), obtaining a device that operates at lower gate voltage values than C-gate OECT. The presence of gold on the gate allowed further modification of the electrical performances by functionalization of the Au-C-gate with different self-assembled monolayers by fast potential-pulse-assisted method. Moreover, we show that the presence in the electrolyte solution of an external redox probe can be used to drive the faradic response of both C- and Au-C-gate OECTs, impacting on the gate potential window that yields effective drain current modulation. The results presented here suggest possible new strategies for controlling the faradic operation regime of OECTs sensors by chemical modification of the gate surface.

Organic electrochemical transistors (OECTs) are finding widespread application in biosensing, thanks to their high sensitivity, broad dynamic range, and low limit of detection. An OECT biosensor requires the immobilization of a biorecognition probe on the gate, or else on the channel, through several, often lengthy, chemical steps. In this work, a fast and straightforward way to functionalize the carbon gate of a fully screen-printed OECT by means of a polydopamine (PDA) film is presented. By chemical immobilization of an amine-terminated single-stranded oligonucleotide, containing the HSP70 promoter CCAAT sequence, on the PDA film, the detection of the complementary DNA strand is demonstrated. Furthermore, the specificity of the developed genosensor is assessed by comparing its response to the fully complementary strand with the one to partially complementary and noncomplementary oligonucleotides. The developed sensor shows a theoretical limit of detection (LOD) of 100 × 10−15 m and a dynamic range over four orders of magnitude. © 2022 The Authors.

Infectious diseases are a potential risk for public health and the global economy. Fast and accurate detection of the pathogens that cause these infections is important to avoid the transmission of the diseases. Conventional methods for the detection of these microorganisms are time-consuming, costly, and not applicable for on-site monitoring. Biosensors can provide a fast, reliable, and point of care diagnostic. Nanomaterials, due to their outstanding electrical, chemical, and optical features, have become key players in the area of biosensors. This review will cover different nanomaterials that employed in electrochemical, optical, and instrumental biosensors for infectious disease diagnosis and how these contributed to enhancing the sensitivity and rapidity of the various sensing platforms. Examples of nanomaterial synthesis methods as well as a comprehensive description of their properties are explained. Moreover, when available, comparative data, in the presence and absence of the nanomaterials, have been reported to further highlight how the usage of nanomaterials enhances the performances of the sensor.

Novel printed electronics are projected to grow and be manufactured in the future in large volumes. In many applications, printed electronics are envisaged as sustainable alternatives to conventional (PCB-based) electronics. One such application is in the semi-quantitative drug detection and point-of-care device called ‘GREENSENSE’ that uses paper-based printed electronics. This paper analyses the carbon footprint of GREENSENSE in order to identify and suggest means of mitigating disproportionately high environmental impacts, labeled ‘sustainability hotspots’, from materials and processes used during production which would be relevant in high-volume applications. Firstly, a life cycle model traces the flow of raw materials (such as paper, CNCs, and nanosilver) through the three ‘umbrella’ processes (circuit printing, component mounting, and biofunctionalization) manufacturing different electronic components (the substrate, conductive inks, energy sources, display, etc) that are further assembled into GREENSENSE. Based on the life cycle model, life cycle inventories are modeled that map out the network of material and energy flow throughout the production of GREENSENSE. Finally, from the environmental impact and sustainability hotspot analysis, both crystalline nanocellulose and nanosilver were found to create material hotspots and they should be replaced in favor of lower-impact materials. Process hotspots are created by manual, lab-, and pilot-scale processes with unoptimized material consumption, energy use, and waste generation; automated and industrial-scale manufacturing can mitigate such process hotspots. © 2023 The Author(s).

There is a profound need in bioprocess manufacturing for low-cost single-use sensors that allow timely monitoring of critical product and production attributes. One such opportunity is screen-printed enzyme-based electrochemical sensors, which have the potential to enable low-cost online and/or off-line monitoring of specific parameters in bioprocesses. In this study, such a singleuse electrochemical biosensor for lactate monitoring is designed and evaluated. Several aspects of its fabrication and use are addressed, including enzyme immobilization, stability, shelf-life and reproducibility. Applicability of the biosensor to off-line monitoring of bioprocesses was shown by testing in two common industrial bioprocesses in which lactate is a critical quality attribute (Corynebacterium fermentation and mammalian Chinese hamster ovary (CHO) cell cultivation). The specific response to lactate of the screen-printed biosensor was characterized by amperometric measurements. The usability of the sensor at typical industrial culture conditions was favorably evaluated and benchmarked with commonly used standard methods (HPLC and enzymatic kits). The single-use biosensor allowed fast and accurate detection of lactate in prediluted culture media used in industrial practice. The design and fabrication of the biosensor could most likely be adapted to several other critical bioprocess analytes using other specific enzymes. This makes this single-use screen-printed biosensor concept a potentially interesting and versatile tool for further applications in bioprocess monitoring. © 2020 by the authors.

Cellulose is the most abundant organic material on our planet which has a key role in our daily life (e.g., paper, packaging). In recent years, the need for replacing fossil-based materials has expanded the application of cellulose and cellulose derivatives including into electronics and sensing. The combination of nanostructures with cellulose nanofibers (CNFs) is expected to create new opportunities for the development of innovative electronic devices. In this paper, we report on a single-step process for the low temperature (<100 °C), environmentally friendly, and fully scalable CNF-templated highly dense growth of zinc oxide (ZnO) nanorods (NRs). More specifically, the effect of the degree of substitution of the CNF (enzymatic CNFs and carboxymethylated CNFs with two different substitution levels) on the ZnO growth and the application of the developed ZnO NRs/CNF nanocomposites in the development of UV sensors is reported herein. The results of this investigation show that the growth and nature of ZnO NRs are strongly dependent on the charge of the CNFs; high charge promotes nanorod growth whereas with low charge, ZnO isotropic microstructures are created that are not attached to the CNFs. Devices manufactured via screen printing/drop-casting of the ZnO NRs/CNF nanocomposites demonstrate a good photo-sensing response with a very stable UV-induced photocurrent of 25.84 µA. This also exhibits excellent long-term stability with fast ON/OFF switching performance under the irradiance of a UV lamp (15 W). 

Low weight, small footprint, and high performances are essential requisites for the implementation of energy storage devices within consumer electronics. One way to achieve these goals is to increase the thickness of the active material layer. In this work, carbonized and graphitized rayon felt, a cellulose-derived material, is used as a three-dimensional current collector scaffold to enable the incorporation of large amount of active energy storage materials and ionic liquid-based gel electrolyte in the supercapacitor devices. PEDOT:PSS, alone or in combination with active carbon, has been used as the active material. Three-dimensional supercapacitors with high per unit area capacitance (more than 1.1 F/cm2) have been achieved owing to the loading of large amount of active material in the felt matrix. Areal energy density of more than 101 μWh/cm2 and areal power density of more than 5.9 mW/cm2 have been achieved for 0.8 V operating voltage at a current density of 1 mA/cm2. A nanographite material was found to be beneficial in reducing the internal serial resistance of the supercapacitor to lower than 1.7 Ω. Furthermore, it was shown that even after 2000 times cycling test, the devices could still retain its performance with at least 88% coulombic efficiency for all the devices. All the materials are readily available commercially, environmentally sustainable and the process can potentially be upscaled with industrial process. © 2022 The Authors.

We describe a composite material for use in electrochemical oxygen reduction. A screen-printed electrode (SPE) was consecutively modified with electrodeposited copper, a Nafion membrane and electropolymerized polyaniline (PANi) to give an electrocatalytic composite of type PANi/Nafion/Cu2O/SPE that displays good electrical conductivity at neutral pH values. It is found that the presence of ammonia causes complex formation with Cu(I), and this causes electroreduction of oxygen to result in an increased cathodic current. The finding was applied to the quantification of ammonium ions in the 1 to 1000 μM concentration range by amperometry at −0.45 V (vs. Ag/AgCl). This Faradaic phenomenon offers the advantage of direct voltammetric detection, one of the lowest known limits of detection (0.5 μM), and high sensitivity (250 mA∙M−1∙cm−2). It was applied to the determination of ammonium ion in human serum where it compared well with the photometric routine approach for clinical analysis using glutamate dehydrogenase. [Figure not available: see fulltext.]

The key step in the construction of efficient and selective analytical separations or sensors is the design of the recognition interface. Biomimicry of the recognition features typically found in biological molecules, using amino acids, peptides and nucleic acids, provides plausible opportunities to integrate biological molecules or their active sites into a synthetic polymeric backbone. Given the basic role of functional amino acids in biorecognition, we focused on the synthesis of polymerizable amino acid derivatives and their incorporation into a polymer-based biohybrid interface to construct generic bioinspired analytical tools. We also utilized polyvinyl alcohol (PVA) as a sacrificial polymer to adjust the porosity of these biohybrid interfaces. The surface morphologies of the interfaces on gold electrodes were characterized by using scanning electron (SEM) and atomic force (AFM) microscopies. The electrochemical behavior of the polymeric films was systematically investigated using differential pulse voltammetry (DPV) to demonstrate the high affinity of the biohybrid interfaces for Cu(II) ions. The presence of macropores also significantly improved the recognition performance of the interfaces while enhancing interactions between the target [Cu(II) ions] and the functional groups. As a final step, we showed the applicability of the proposed analytical platform to create a Cu(II) ion-mediated supramolecular self-assembly on a quartz crystal microbalance (QCM) electrode surface in real time.