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On-site detection of multiple small-molecule analytes in complex sample matrixes would be highly valuable for diverse biosensing applications. Paper electrochemical devices (PEDs) offer an especially appealing sensing platform for such applications due to their low cost, portability, and ease of use. Using oligonucleotide-based aptamers as biorecognition elements, we here for the first time have developed a simple, inexpensive procedure for the fabrication of aptamer-modified multiplex PEDs (mPEDs), which can robustly and specifically detect multiple small molecules in complex samples. These devices are prepared via an ambient vacuum filtration technique using carbon and metal nanomaterials that yields precisely patterned sensing architecture featuring a silver pseudo-reference electrode, a gold counter electrode, and three gold working electrodes. The devices are user-friendly, and the fabrication procedure is highly reproducible. Each working electrode can be readily modified with different aptamers for sensitive and accurate detection of multiple small-molecule analytes in a single sample within seconds. We further demonstrate that the addition of a PDMS chamber allows us to achieve detection in microliter volumes of biological samples. We believe this approach should be highly generalizable, and given the rapid development of small-molecule aptamers, we envision that facile on-site multi-analyte detection of diverse targets in a drop of sample should be readily achievable in the near future.

This paper introduces a novel potential-resolved paper-based biosensor for simultaneous detection of multiple microRNAs (miRNAs) (taking miRNA-155 and miRNA-126 as examples) based on the bipolar electrode (BPE) electrochemiluminescence (ECL) strategy. The proposed multiple-channel paper-based sensing microfluidic platform was prepared by wax-printing technology, screen-printing method, and in situ Au nanoparticles (AuNPs) growth to form hydrophilic areas, hydrophobic boundaries, waterproof electronic bridge, driving electrode regions, and parallel bipolar electrode regions. CdTe quantum dots (QDs)-H2 and Au@g-C3N4 nanosheets (NSs)-DNA1 were used as dual electrochemiluminescence signal probes, and carboxylated Fe3O4 magnetic nanoparticles existed as carriers. CdTe QDs-H2/S2O82- and Au@g-C3N4 NSs-DNA1/S2O82- could exhibit two strong and stable ECL emissions at a drive voltage of 9 and 12 V, respectively, which can be used as effective potential-resolved signal tags. In addition, the proposed three-dimensional (3D) DNA nanomachine model and the target miRNA cycle strategy were used to achieve double amplification of electrochemiluminescence intensity. More importantly, the combination of the bipolar electrode system and the potential-resolved multitarget electrochemiluminescence method can greatly reduce the spatial interference between substances. The prepared ECL biosensor showed a favorable linear response for the detection of miRNA-155 and miRNA-126 with relatively low detection limits of 5.7 and 4.2 fM, respectively. With excellent sensitivity, the strategy may provide an efficient method for clinical application, especially in detection of trace multiple targets.

A novel 3D paper-based microfluidic screen-printed electrode (SPE) composed of two layers was constructed by photolithography and screen-printing technology. Aldehyde functionalized hydrophilic zone of the counter and reference electrodes layer was prepared for glucose oxidase immobilization. Highly conductive Prussian blue deposited reduced graphene oxide-tetraethylene pentamine (rGO-TEPA/PB) modified paper working electrode layer can be used as an electrochemical sensitive membrane for quantitative detection of hydrogen peroxide (H2O2), which was the enzyme-catalyzed reaction product. Therefore, this 3D paper-based microfluidic electrochemical biosensor can be used for quantitative detection of glucose. Under optimum conditions, the proposed biosensor can be used for quantitative determination of glucose over a wide linear range of 0.1 mM∼25 mM with detection limit of 25 μM. Finally, the 3D paper-based microfluidic electrochemical biosensor was applied to determine glucose in human sweat and blood, and the obtained results were in good consistency with values measured by Roche's blood glucose meter. In addition, the proposed 3D paper-based electrochemical device showed good repeatability, stability, and anti-interference, which would be of great potential to monitor glucose in complex biological fluids.

Cobalt(ii) phthalocyanine (CoPc) was suspended in aqueous medium and the colloidal system was used as catalyst for the electrochemical determination of hydrogen peroxide on paper-based electrodes modified with carbon nanomaterials. H2O2 was oxidised at 0.275 V vs. Ag pseudoreference electrode. This system was adapted to develop a glucose sensor with glucose oxidase immobilized on the cellulose electrode. CoPc suspended nanoparticles acted as nanoenzyme mimicking peroxidase activity and were combined with different carbon nanomaterials to form hybrids with optimised catalytic performance. GO-CoPc paper-based electrodes yielded the best results with a linear range of ∼12 μM to 49 mM for H2O2 and 0.1 mM to 1 mM for glucose. Glucose was determined in physiological serum and juice samples with recoveries of 93.3 and 94.2% respectively. CoPc could replace HRP for the catalytic sensing of H2O2, without the need to be dissolved. This material can be used in situ in a simple protocol with other nanomaterials for electrode modification. The sensor described has the advantage of easy preparation, using the catalyst in colloidal form, long term stability, and versatility to be adapted to other low cost and disposable enzymatic systems.

The development of actuators for power sources is essential for the efficient manipulation of fluids in microfluidics systems. In this work, a capacitor-type three-layer paper actuator was fabricated by sandwiching a polyelectrolyte layer between two films of poly(3,4-ethylenedioxythiophene) doped with poly(4-styrenesulfonate) (PEDOT/PSS). The paper actuator exhibited stable large electromechanical deformations in bilateral symmetry under alternating square-wave electric field. The actuation properties were examined in a function of voltage (±0.5, ±1, ±1.5, ±2, and ±2.5 V) and frequency (1, 0.5, 0.2, and 0.05 Hz). In addition, the PEDOT/PSS electrode films with different thicknesses were prepared, and the effects of actuator thickness on actuation properties were examined. As a result, it was found that the actuator displacement increased considerably with reducing actuator thickness. In addition, the actuator with a thickness of 48 μm demonstrated a maximum displacement of 5.8 mm at a voltage of 1.5 V and a frequency of 0.05 Hz. The proposed actuator can be potentially used in the development of power sources for micropumps and check valves of microfluidic devices.

In the present article we report a new hybrid microfluidic device (hyFlow) comprising a disposable paper electrode and a three-dimensional (3D) printed plastic chip for the electrochemical detection of a magnetic bead-silver nanoparticle (MB-AgNP) bioconjugate. This hybrid device evolved due to the difficulty of incorporating micron-scale MBs into paper-only fluidic devices. Specifically, paper fluidic devices can entrap MB-containing conjugates within their cellulose or nitrocellulose fiber matrix. The hyFlow system was designed to minimize such issues and transport MB conjugates more efficiently to the electrochemical detection zone of the device. The hyFlow system retains the benefit of fluid transport by pressure-driven flow, however, no pump is required for its operation. The hyFlow device is capable of detecting either pre-formed MB-AgNP conjugates or conjugates formed in-situ formation. The detection limit of AgNPs using this device is 12 pM, which represents just 22 AgNPs per MB.

Despite substantial advances in sensing technologies, the development, preparation, and use of self-testing devices is still confined to specialist laboratories and users. Decentralized analytical devices will enormously impact daily lives, enabling people to analyze diverse clinical, environmental, and food samples, evaluate them and make predictions to improve quality of life, particularly in remote, resource-scarce areas. In recent years, paper-based analytical tools have attracted a great deal of attention; the well-known properties of paper, such as abundance, affordability, lightness, and biodegradability, combined with features of printed electrochemical sensors, have enabled the development of sustainable devices that drive (bio)sensors beyond the state of the art. Their blindness toward colored/turbid matrices (i.e., blood, soil), their portability, and the capacity of paper to autonomously filter/purge/react with target species make such devices powerful in establishing point-of-need tools for use by non-specialists. This protocol describes the preparation of a voltammetric phosphate sensor and an amperometric nerve agent biosensor; both platforms produce quantitative measurements with currents in the range of microamperes. These printed strips comprise three electrodes (graphite for working and counter electrodes and silver/silver chloride (Ag/AgCl) for the reference electrode) and nanomodifiers (carbon black and Prussian blue) to improve their performance and specificity. Depending on analytical need, different types of paper (filter, office) and configurations (1D, 2D, 3D) can be adopted. The protocol, based on the use of cost-effective manufacturing techniques such as drop casting (to chemically modify the substrate surface) and wax/screen printing (for creating the channels and electrodes), can be completed in

This paper demonstrates a simple-in-struct- ure, cost-effective, and environment-friendly Microfluidic Paper-based Analytical Device for Microbial Biofuel Cell ( $\mu $ PAD-MBFC). It consists of a microchannel with biofuel cell (Escherichia.Coli) and an oxidant (aerated tap water) flowing co-parallelly over Multiwalled Carbon Nanotube (MWCNT)-based Bucky Paper (BP) electrodes using a self-capillary and co-laminar flow mechanism. The electrochemical studies, such as open circuit potential (OCP) and polarization were evaluated using a potentiostat. Various volumetric bacterial studies were also carried out to find out the best suitable optimal bacterial volume. Subsequently, the morphological and detailed element composition study of electrode surface was performed using scanning electron microscopy (SEM) and energy dispersive spectroscopy (EDS) techniques. This well-designed portable $\mu $ PAD-MBFC yields a maximum power density of 4 $\mu \text{W}$ /cm2 ( $20~\mu \text{A}$ /cm2) at 0.405 V over $200~\mu \text{l}$ of culture and leveraging to its long-lasting potential to operate miniaturized microelectronics sensors and portable devices.

RATIONALE Paper spray (PS) has been developed as a method of choice for point-of-care analysis in many real cases, where its applications can be further expanded with delicate high-throughput design. To achieve this goal, we developed a new PS regime, with the assembly of an induced high voltage into the ion source. Compared with regular DC high voltage, the newly developed setup is capable of high-throughput, simple configuration and rapid switching between individual papers without complicated electric/mechanic design. METHODS A device of high-throughput induced PS (IPS) was designed by using a two-dimensional (2D) rotating platform equipped with a circular glass plate. The paper substrate was placed on the circular glass plate and separated from the electrode. The method avoids physical contact between the electrode and the sample. Charged droplets were generated at the paper tip once an induced high voltage was applied to a wet paper. RESULTS A relatively rapid analytical speed of 2.6 s per sample was achieved via IPS-MS. Rapid quantification of amitriptyline (AMT) in complicated matrices was obtained within 1 min using an isotope internal standard method. Limits of detection for AMt in urine, FBS and blood were calculated to be 1.04, 0.84 and 1.33 ng/mL, respectively. In addition, high-throughput IPS-MS can be used for chemical reaction monitoring. CONCLUSIONS We have demonstrated the versatility of high-throughput IPS-MS in ambient ionization, which successfully simplified the experimental installation and facilitated the experimental operation. Therefore, we believe that high-throughput IPS-MS analysis will be widely used for discovering drugs and screening reactions, and the present design has the potential for applications in paper chip-MS analysis.

Paper-based strain sensors have attracted attention as a cost-effective and environmentally friendly approach to wearable electronic devices. This paper proposes a paper-based strain sensor created solely using hand-painting, which is a simple, equipment-free process utilized in green electronics. Commercial printing paper is coated with polydimethylsiloxane diluted with heptane, which provides moisture resistance and mechanical robustness while increasing the hydrophobicity of the surface. The electrodes and conduction channels are fabricated using a pencil for graphite deposition and a brush for the deposition of tin-doped indium oxide nanoparticles, respectively. With a gauge factor of 41.98 in tensile strain tests and 21.36 in compressive strain tests, our strain sensor exhibits a good sensitivity that is similar to that of previously reported paper-based sensors. We also demonstrate that our proposed strain sensor can be used as a weak motion detection device for humans and robots.

In this work, a self-circulation oxygen-hydrogen peroxide-oxygen (O2-H2O2-O2) system with photogenerated electrons as fuel and highly active hemin monomers as operators was engineered for ultrasensitive cathode photoelectrochemical bioassay of microRNA-141 (miRNA-141) using a stacked sealed paper device. During the circulation, the photogenerated electrons from BiVO4/Cu2O photosensitive structures assembled on a reduced graphene oxide paper electrode first reduced the electron acceptors (dissolved O2) to H2O2, which was then catalytically decomposed by hemin monomers to generate O2 again. The regenerated O2 continued to be reduced, which made O2 and H2O2 stuck in the infinite loop of O2-H2O2-O2 accompanied by the fast consumption of photogenerated electrons, generating an amplified photocurrent signal. When a target existed, a duplex-specific nuclease-induced target recycling reaction with dual trigger DNA probes as the output was performed to initiate the assembly of bridge-like DNA nanostructures, which endowed the self-circulation system with dual destruction functions as follows. (i) Reduced fuel supply: the assembled DNA bridges acting as a negatively charged barrier prevented the photogenerated electrons from participating in the O2 reduction to H2O2. (ii) Incapacitation of operators: DNA bridging induced the dimerization of hemin monomers linked on the DNA hairpins to catalytically inactive hemin dimers, leading to the abortive regeneration of O2. These destruction functions resulted in the circulation interruption and a remarkably decreased photocurrent signal. Thus, the developed cathode photoelectrochemical biosensing platform achieved ultrasensitive miRNA-141 detection with a linear range of 0.25 fM to 1 nM and a detection limit of 83 aM, and it also exhibited high accuracy, selectivity, and practicability.

Electrochemical aptamer-based (E-AB) sensors offer a powerful and general means for analyte detection in complex samples for various applications. Paper-based E-AB sensors could enable portable, low-cost, and rapid detection of a broad range of targets, but it has proven challenging to fabricate suitable three-electrode systems on paper. Here, we demonstrate a simple, economic, and environmentally-friendly strategy for fabricating aptamer-modified paper electrochemical devices (PEDs) via ambient vacuum filtration. The electrode material, shape, size, and thickness of the three-electrode PED system can be fully customized. We developed aptamer-modified PEDs that enable sensitive and specific detection of small molecules in minimally processed biosamples. The sensitivity and stability of the PEDs is comparable to E-AB sensors based on commercial gold electrodes. We believe our fabrication strategy can lead to the development of high performance PEDs that enable on-site detection of a variety of analytes, simplifying the development of portable sensors for real-world applications.

Pencils and papers are ubiquitous in our society and have been widely used for writing and drawing, because they are easy to use, low-cost, widely accessible, and disposable. However, their applications in emerging skin-interfaced health monitoring and interventions are still not well explored. Herein, we report a variety of pencil–paper-based on-skin electronic devices, including biophysical (temperature, biopotential) sensors, sweat biochemical (pH, uric acid, glucose) sensors, thermal stimulators, and humidity energy harvesters. Among these devices, pencil-drawn graphite patterns (or combined with other compounds) serve as conductive traces and sensing electrodes, and office-copy papers work as flexible supporting substrates. The enabled devices can perform real-time, continuous, and high-fidelity monitoring of a range of vital biophysical and biochemical signals from human bodies, including skin temperatures, electrocardiograms, electromyograms, alpha, beta, and theta rhythms, instantaneous heart rates, respiratory rates, and sweat pH, uric acid, and glucose, as well as deliver programmed thermal stimulations. Notably, the qualities of recorded signals are comparable to those measured with conventional methods. Moreover, humidity energy harvesters are prepared by creating a gradient distribution of oxygen-containing groups on office-copy papers between pencil-drawn electrodes. One single-unit device (0.87 cm(2)) can generate a sustained voltage of up to 480 mV for over 2 h from ambient humidity. Furthermore, a self-powered on-skin iontophoretic transdermal drug-delivery system is developed as an on-skin chemical intervention example. In addition, pencil–paper-based antennas, two-dimensional (2D) and three-dimensional (3D) circuits with light-emitting diodes (LEDs) and batteries, reconfigurable assembly and biodegradable electronics (based on water-soluble papers) are explored.

We report for the first time a highly sensitive and rapid quantitative method for the detection of Salmonella Typhimurium (S. Typhimurium) using a conductive immunosensor on a paper-based device (PAD). S. Typhimurium monoclonal antibodies (MA) were first immobilized on a paper-based device and then captured by S. Typhimurium. After an immunoreaction on the device, the polyclonal antibody-colloidal gold conjugate (PA-AuNPs) was dropped to bind with S. Typhimurium. After a complete sandwich reaction, a dark red color appeared on the paper-based device, which can be observed by the naked eye for a rapid screening test. The electrical conductivity of PA-AuNPs between the screen-printed electrodes on the paper-based device was also measured for an accurate quantitative analysis. The electrical conductivity correlated well with the concentration of S. Typhimurium, which was controlled by the amount of S. Typhimurium attached to the polyclonal antibody-colloidal gold conjugate. The device showed a linear correlation for the concentration of the S. Typhimurium in the range of 10–108 CFU mL−1 in a logarithmic plot, with an R2 value of 0.9882 and a limit of detection (LOD) as low as 10 CFU mL−1. This simple, highly sensitive, and rapid method for the S. Typhimurium detection was successfully performed within 30 min, and it can be developed into small portable measuring devices in order to facilitate preliminary screening tests.

A new class of biosensing transducer based on alternating-current electroluminescent (ACEL) display is demonstrated. Unlike conventional ACEL displays where they have been rigidly used in flexible screens and advertising applications, here, the display is integrated with immunoassay and functioned as an optical transducer. Taking advantage of the reversed ACEL architecture, the display can be simply fabricated on an unconventional paper material without requiring the transparent indium tin oxide (ITO) electrode. The sensing mechanism relies on the promoted electronic conduction from the immunocomplex formation between immobilized antibody, antigen, and nanoparticle labeled antibody. As a result, the electroluminescence could be triggered off instantaneously. To demonstrate the device effectiveness, C-reactive protein (CRP), a particular biomarker of an inflammatory process and cardiovascular disease, is chosen as a model analyte in this work. Additionally, the applicability of the proposed platform is proved efficacious in human serums, showing negligible interference from nontargeting proteins. The sensing display is also capable of performing multiple assays (up to 8) within a single device. This bio-optoelectronic device represents a straightforward yet highly sensitive approach. This ACEL transducer is believed to explore new possibilities for biosensing and exploit in point-of-care testing.

Norovirus is one of the leading causes of gastroenteritis, acute vomiting, intense diarrhoea, acute pain in the stomach, high fever, headaches, and body pain. Conventional methods of detection gave us very promising results but had disadvantages such as low sensitivity, cost ineffectiveness, reduced specificity and selectivity, etc. Therefore, biosensors can be a viable alternative device which can overcome all setbacks associated with the conventional method. An electrochemical sensor based on oxidized graphitic carbon nitride (Ox-g-C3N4) modified electrochemical paper-based analytical device (ePAD) was fabricated for the detection of norovirus DNA. The synthesized Ox-g-C3N4 nanosheets were characterized by field emission scanning electron microscopy (FESEM), X-ray Diffraction (XRD), UV-Vis spectroscopy and X-Ray Photoelectron Spectroscopy. The capture probe DNA (PDNA) modified electrodes were characterized by cyclic voltammetry (CV) and differential pulse voltammetry (DPV). These two characterization techniques were also employed to find the optimal scan rate, response time and temperature of the fabricated sensor. The fabricated biosensor showed a limit of detection (LOD) of 100 fM. Furthermore, the specificity of the reported biosensor was affirmed by testing the response of capture probe DNA with oxidized graphitic carbon nitride (PDNA/Ox-g-C3N4) modified ePAD on the introduction of a non-complimentary DNA. The fabricated ePAD sensor is easy to fabricate, cost effective and specific, and requires a minimum analysis time of 5 s.

Advances in cutting-edge technologies including nanotechnology, micmfluidics, electronic engineering, and material science have boosted a new era in the design of robust and sensitive biosensors. In recent years, carbon black has been re-discovered in the design of electrochemical (bio)sensors thanks to its interesting electroanalytical properties, absence of treatment requirement, cost-effectiveness (c.a. 1 (sic)/Kg), and easiness in the preparation of stable dispersions. Herein, we present an overview of the literature on carbon black-based electrochemical (bio)sensors, highlighting current trends and possible challenges to this rapidly developing area, with a special focus on the fabrication of carbon black-based electrodes in the realisation of sensors and biosensors (e.g. enzymatic, immunosensors, and DNA-based).

Paper-based carbon working electrodes were modified with mercury or bismuth films for the determination of trace metals in aqueous solutions. Both modification procedures were optimized in terms of selectivity and sensitivity for the determination of different heavy metals, aiming their simultaneous determination. Cd (II), Pb (II) and In (III) could be quantified with both films. However, Cu (II) could not be determined with bismuth films. The modification with mercury films led to the most sensitive method, with linear ranges between 0.1 and 10 &micro, g/mL and limits of detection of 0.4, 0.1, 0.04 and 0.2 &micro, g/mL for Cd (II), Pb (II), In (III) and Cu (II), respectively. Nevertheless, the bismuth film was a more sustainable alternative to mercury. Tap-water samples were analyzed for the determination of metals by standard addition methodology with good accuracy, by using a low-cost and easily disposable paper-based electrochemical platform. This system demonstrated its usefulness for monitoring heavy metals in water.

Treatment for cancer depends on the type of cancer, and the stage or its development, and thus the need for point-of-care technology that can allow rapid and precise detection of biomarkers is increasing. Here, we present a simple on chip electrical detection of Alpha-fetoprotein (AFP). We rely on using a novel peptide modified plastic-paper microfluidic chips to perform efficient and specific impedimetric detection of AFP in human serum. The chips are prepared from a lower sheet of plastic and upper layer of cellulose chromatography paper modified with silver-20 wt% graphene printed electrodes. Diphenylalanine (FF) was proposed to involve in detection zone of the fabricated microchips in order to improve the sensing performance and the stability of immobilized antibodies according to amine-aldehyde reaction. The target protein is captured on the surface of microchips using specific monoclonal antibodies and the electrical response of the chip is monitored in the presence and absence of different concentrations of AFP. The influence of several parameters including the material types for screen printing of electrodes, FF concentrations, solvent and pH of FF solution on electrical response and cellulose fibers morphology was explored. The impedance measurements of AFP on the fabricated microchip in the optimized parameters exhibited a detection limit of 1 and 10 ng ml-1 in PBS and plasma, respectively. This platform developed here can be adopted to develop systems for rapid detection of biomarkers using portable electric devices.

This paper establishes a membraneless, co-laminar flow-based approach to develop a cost-effective microfluidic paper-based analytical device for enzymatic biofuel cell ( $\mu $ PAD-EBFC). The developed $\mu $ PAD-EBFC supporting the self-capillary fluid transport action consists of Y-shaped paper microchannel with the fuel (glucose) and oxidant (O2) streaming in parallel over carbon nanotube-based bucky paper electrodes modified with biocompatible electrocatalytic enzymes, such as glucose oxidase and laccase without any additional redox cofactor. The electrochemical performance for the modified bioelectrodes, i.e., electrocatalytic oxidation and reduction reaction, was carried out using linear sweep voltammetry, cyclic voltammetry, and open circuit potential. The overall performance of $\mu $ PAD-EBFC was evaluated using the polarization studies. Subsequently, the catalytic activity of enzymes on the electrode surface was validated by the scanning electron microscope. This simple and portable $\mu $ PAD-EBFC can generate the maximum power density to the order of $100~\mu \text{W}$ /cm2 ( $600~\mu \text{A}$ /cm2) at 0.505 V over prolonged durations of around 50 h. Hence, the presented $\mu $ PAD-EBFC shows good power density and stability, leading to its strong potential to power miniaturized microelectronics devices and sensors.

Nowadays, environmentally friendly synthesis pathways for preserving the environment and minimizing waste are strongly required. Herein, we propose filter paper as a convenient scaffold for chemical reactions. To demonstrate this novel approach, Prussian Blue Nanoparticles (PBNPs) were synthesized on filter paper by utilizing few μL of its precursors without external inputs, i.e. pH, voltage, reducing agents, and without producing waste as well. The functional paper, named “Paper Blue”, is successfully applied in the sensing field, exploiting the reduction of hydrogen peroxide at low applied potential. The eco-designed “Paper Blue” was combined with wax- and screen-printing to manufacture a reagentless electrochemical point-of-care device for diabetes self-monitoring, by using glucose oxidase as the biological recognition element. Blood glucose was linearly detected for a wide concentration range up to 25 mM (450 mg/dL), demonstrating its suitability for management of diabetes and glucose-related diseases. The Paper Blue-based biosensor demonstrated a correlation coefficient of 0.987 with commercial glucose strips (Bayer Contour XT). The achieved results demonstrated the effectiveness of this approach, which is also extendible to other (bio)systems to be applied in catalysis, remediation, and diagnostics.

We propose a paper solar cell based on carbon nanotube (CNT)-composite papers. To fabricate this cell, we use dye-sensitized solar cells (DSCs) for generating power through the redox reaction of dyes in conjunction with CNT-composite papers, which are composite materials containing CNTs and pulp (raw paper material) that can be fabricated easily by using a method based on the Japanese washi papermaking technique. The demand for CNT applications is expected to increase due to their high conductivity and metallic or semiconducting characteristics. This CNT-composite paper can also have metallic or semiconducting characteristics based on the contained CNTs in the composite paper. We previously fabricated a DSC that generates electricity by using CNT-composite papers stacked in a typical DSC structure. However, the conversion efficiency of this DSC was just 0.188%, which is not practical. To overcome this low power generation issue, we tried improving the DSC structure by applying electrodes to the CNT-composite papers in grid patterns for efficient current collection and applying an optimally mixed dye for efficient electron excitation. Results showed that the conversion efficiency improved to 0.58%. Moreover, we demonstrated that using a mixed dye can improve the conversion efficiency of the paper DSC. We expect these types of CNT-composite papers to be used as material for new DSCs.

The low solubility of gas molecules in aqueous solutions has limited the power density output of enzymatic biofuel cells. Herein, a single-liquid miniature glucose–O2 fuel cell was constructed by using gas diffusion electrodes, which were prepared by immobilizing glucose oxidase (GOx) or laccase (Lac) modified on a porous structured carbon paper (CP). Due to the fast and direct O2 diffusion from air to the active sites of the immobilized enzyme through the pores of the CP anode/cathode with controlled wettability, the maximum power output densities dramatically increased to 9.64 μW cm−2 at 0.43 V and 53.0 μW cm−2 at 0.45 V for the cell in 5 mM glucose and after exposing the cell to air or O2 atmosphere, respectively. Interestingly, the resulting single-liquid cell could harvest power from human serum operating at a maximum power density of 49.0 μW cm−2 at 0.2 V. The biofuel cell fabricated by the gas diffusion electrodes displayed advantages such as high output power density, low cost and high ‘on-chip’ integrability and miniaturization, which suggest its great potential for implantable self-powered sensors and for many future applications.

Aiming to overcome the obstacles of power supply requirement and chip usefulness in practice, a low-cost and convenient portable electrochemical sensing device is introduced for the first time, featuring bipolar electrode system, LED read-out, laminated paper-based devices, and low-voltage button cells. The electric circuits of this practical device are constructed on laminating films with copper and conductive carbon tapes, and the reservoirs facilitating chemical reactions are made with chromatography paper. The device is sensitive to electrochemical responses, validated by the demonstrative hydrogen peroxide and enzyme-assisted glucose detection. The business-card-size chip achieves sensitive analyte detection by naked eyes as well as further image processing in both laboratory samples and human serum samples testing, featuring detection limit as low as 1.79 μM and a dynamic range from 10 μM to 10 mM. This new practical design of point-of-care sensing chip entails the properties of facile fabrication, simple usage, high robustness, low power consumption, and accurate sensing showing the attainability of fabricating a useful and portable analytical device.

In this paper, a new and facile method for the electrochemical determination of l-tyrosine was designed. First, 3-mercaptopropyl trimethoxysilane-functionalized silica nanoparticles were added to a paper disc. Then, the banana peel tissue and the mediator potassium hexacyanoferrate were dropped onto the paper, respectively. The modified paper disc was placed on the top of the graphite screen printed electrode and electrochemical characterization of this biosensor was studied by cyclic voltammetry and electrochemical impedance spectroscopy methods. The effective parameters like pH, banana peel tissue percentage, and the amount of mediator loading were optimized. l-tyrosine measurements were done by differential pulse voltammetry with a little sample (3 μL) for analysis. The biosensor showed a linear response for l-tyrosine in the wide concentration range of 0.05-600 μM and a low detection limit about 0.02 μM because of the co-catalytic effect of enzyme and nanoparticles. The stability of the biosensor and its selectivity were evaluated. This biosensor was applied for the voltammetric determination of l-tyrosine in the blood plasma sample. The results of the practical application study were comparable with the standard method (HPLC). In conclusion, a simple, inexpensive, rapid, sensitive and selective technique was successfully applied to the l-tyrosine analysis of the little samples.

Although significant technological advancements have been made in the development of analytical biosensor chips for detecting bacterial strains (E. coli, S. Mutans and B. Subtilis), critical requirements i.e. limit of detection (LOD), fast time of response, ultra-sensitivity with high reproducibility and good shelf-life with robust sensing capability have yet to be met within a single sensor chip. In order to achieve these criteria, we present an electrically-receptive thermally-responsive (ER-TR) sensor chip comprised of simple filter paper used as substrate coated with composite of poly(N-isopropylacrylamide) polymer (PNIPAm) - graphene nanoplatelet (GR) followed by evaporation of Au electrodes for capturing both Gram-positive (S. mutans and B. subtilis) and Gram-negative (E. coli) bacterial cells in real-time. Autoclave water, tap water, lake water and milk samples were tested with ER-TR chip with and without bacterial strains at varying concentration range 101-105 cells/mL. The sensor was integrated with in-house built printed circuit board (PCB) to transmit/receive electrical signals. The interaction of E. coli, S. mutans and B. subtilis cells with fibers of PNIPAm-GR resulted in a change of electrical resistance and the readout was monitored wirelessly in real-time using MATLAB algorithm. Finally, prepared ER-TR chip exhibited the reproducibility of 85-97% with shelf-life of up to four weeks after testing with lake water sample.

This work reports a microfabricated electrochemical paper-based analytical device (ePAD) for the voltammetric determination of DNA. The device is patterned by wax-printing on paper and features a circular assay zone connected to an inlet zone and a sink via grooved microfluidic channels for accelerated flow rate. An electrochemical cell with integrated electrodes is formed on the reverse side of the paper by sputtering of thin metal films (Sn, Pt and Ag as the working, counter and reference electrode, respectively). Proof-of-principle of the ePAD for biosensing is demonstrated for a DNA assay involving attachment of capture DNA, hybridization with biotinylated target oligonucleotide and labeling with streptavidin-conjugated CdSe/ZnS quantum dots (QDs). After the acidic dissolution of the QDs, the released Cd(II) is quantified by anodic stripping voltammetry (ASV) at the Sn-film working electrode. Thanks to the synergistic effects of QDs amplification, the inherent sensitivity of ASV and the excellent detection capabilities of the Sn-film working electrode for Cd(II), the target DNA can be detected at levels as low as 0.11 pmol L

A novel recognition element of molecularly imprinted films (MIFs) was synthesized by wet phase inversion (WPI) on the surface of Ti/TiO2 electrode for highly selective and sensitive electrochemical detection of bisphenol A (BPA). The Ti/TiO2/MIFs sensor was constructed by casting the precursor poly(acrylonitrile-co-acrylic acid) (p(AN-co-AA)) in dimethyl sulfoxide containing template molecule BPA onto the electrode and then immersing into water, resulting in simultaneous p(AN-co-AA) precipitation and BPA imprinting via the facile WPI. The imprinted sites could selectively rebind BPA through hydrogen bonding and hence lead to the equalizing current increase in amperometric detection, by which the BPA could be sensed electrochemically. Accordingly, the Ti/TiO2/MIFs sensor offered a favorable linearity within the wide range over five orders of magnitude (4.4nM-0.13mM), and a low detection limit down to 1.3nM. Excellent recognition selectivity for BPA was also attained over its analogues. Furthermore, this sensor was successfully applied to detect BPA in seawater and paper cup samples, and high recoveries were 86-110% with low relative standard deviations of 1.3-3.2%. By using BPA as a model, the MIFs-based method may provide a facile, rapid, and cost-effective way for ultrasensitive electrochemical measurements of various targeted compounds with good applicability to WPI.

Paper-based microfluidic devices with screen-printed electrodes (SPEs) for electrochemical sensing are popular for low-cost point-of-care diagnostics. The electroactive sensing area in these devices is always the irregular, bottom-SPE surface which is in contact with the analyte flowing within the paper substrate. Unfortunately, this results in an electroactive area which varies widely from sensor to sensor. In this paper, we present a three-dimensional paper-based analytical device with a hollow 3D fluid reservoir which allows for use of a more uniform top-SPE surface as the electroactive sensing area. The use of this isolated reservoir eliminates the need for dielectric inks used in conventional SPEs on paper. Our sensors are fabricated using a combination of wax-printing, screen-printing and simple folding via a cleanroom free process without the need for expensive equipment. Additionally, for the first time, we demonstrate an electrochemical paper-based analytical device with a custom designed potentiostat integrated circuit (IC) as a miniaturized reader. The versatility of the sensor is demonstrated through voltammetric, amperometric and potentiometric measurements of important biochemical analytes such as dopamine, glucose and pH. The 3D ePAD together with a custom CMOS potentiostat demonstrates a low-cost, versatile, self-contained system suitable for point-of-care diagnostic devices.

Prompt development of electronic devices and sensors raised the requirement for design/fabrication of advanced energy sources capable of providing considerable amount of energy for consuming platforms through practical nanotechnological approaches. For this aim, we have developed a highly active 2D nanostructure consisted of reinforced conductive polypyrrole (PPy) with decorated reduced graphene oxide (rGO) with hybrid metal oxide complex of Ni/W (PPy-G-Ni-W) toward supercapacitor applications. The hybrid 2D platform showed remarkable specific capacitance of 597 F.g(-1) and 557 F.g(-1) using CV and GCD analyses, respectively, through using three-electrode system. The developed supercapacitor exhibited fantastic stability upon maintaining 98.2% of its total performance after 5000 charge-discharge cycles. Likewise, the applicable two-electrode device using same electrode configurations composed of PPy-G-Ni-W//PPy-G-Ni-W showed specific capacitances of 361 F.g(-1) and 342 F.g(-1) at scan rate and current density of 2 mV.s(-1) and 0.5 A.g(-1) using CV and GCD techniques, respectively. Outcome of optimum supercapacitance configuration consisted of two-electrode system exhibits ideal energy density of 14.4 Wh.kg(-1) at power density of 275 W.kg(-1). More importantly, the device preserved 96.4% of its total specific capacitance after 5000 charge-discharge cycles which highlighting the excellent capacitive capability along with ultra-stability of the developed platform toward real energy applications.

An electrochemical immunofiltration analysis was introduced into microfluidic paper-based analytical devices (μPADs) for the first time, which was based on photolithography and screen-printing technology. The hydrophilic test zones of the aldehyde-functionalized screen-printed electrodes (SPEs) were biofunctionalized with capture antibodies (Ab1). A sensitive immune detection method was developed by using primary signal antibody functionalized gold nanoparticles (GNPs/Ab2) and alkaline phosphatase conjugated secondary antibody (ALP-IgG). Differential pulse voltammetry (DPV) was performed to detect the electrochemical response. The microfluidic paper-based electrochemical immunosensor (μ-PEI) was optimized and characterized for the detection of human chorionic gonadotropin (HCG), a model analyte, in a linear range from 1.0mIUmL-1 to 100.0 IU mL-1 with a detection limit of 0.36mIUmL-1. Additionally, the proposed μ-PEI was used to test HCG in real human serum and obtained satisfactory results. The disposable, efficient, sensitive and low-cost μ-PEI has exhibited great potential for the development of point-of-care testing (POCT) devices that can be applicated in healthcare monitoring.

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.

A novel paper-based potentiometric sensor with an enhanced response for the detection of glucose in biological fluids is presented. The electrode consists on platinum sputtered on a filter paper and a Nafion membrane to immobilize the enzyme glucose oxidase. The response obtained is proportional to the logarithm of the concentration of glucose, with a sensitivity of -119 +/- 8 mV.decade(-1), a linear range that spans from 10(-4)M to 10(-2.5) M and a limit of detection of 10(-4.5) M of glucose. It is shown that Nafion increases the sensitivity of the technique while minimizing interferences. Validation with human serum samples shows an excellent agreement when compared to standard methods. This approach can become an interesting alternative for the development of simple and affordable devices for point of care and home-based diagnostics.

We describe the design and characteristics of a paper-based analytical device for analyte concentration enrichment. The device, called a hybrid paper-based analytical device (hyPAD), uses faradaic electrochemistry to create an ion depletion zone (IDZ), and hence a local electric field, within a nitrocellulose flow channel. Charged analytes are concentrated near the IDZ when their electrophoretic and electroosmotic velocities balance. This process is called faradaic ion concentration polarization. The hyPAD is simple to construct and uses only low-cost materials. The hyPAD can be tuned for optimal performance by adjusting the applied voltage or changing the electrode design. Moreover, the throughput of hyPAD is 2 orders of magnitude higher than that of conventional, micron-scale microfluidic devices. The hyPAD is able to concentrate a range of analytes, including small molecules, DNA, proteins, and nanoparticles, in the range of 200−500-fold within 5 min.

The demand for high-quality graphene for electronic applications is increasing due to its high carrier mobility and electrical conductivity. In this connection, printing technology is a reliable method towards the fabrication of conductive, disposable graphene-based electrode for low-cost sensor application. Herein, we aimed to report the synthesis of high-quality graphene nanosheets obtained by electrochemical exfoliation of biomass-derived from corn cob. The conductive ink was prepared from this exfoliated graphene and was utilized for the preparation of paper-based graphene electrode towards double stranded DNA (dsDNA) sensor application. This paper, based graphene electrode opens the possibility of direct electrochemical analysis of analyte without any sample preparation. In this study, two irreversible oxide peaks were obtained from paper-based printed graphene electrode, corresponds to oxidation of guanine (G) and adenine (A) of dsDNA in the linear range of 0.2 pg mL−1 to 5 pg mL−1 with the detection limit of 0.68 pg mL−1 and the sensitivity of 0.00656 mA pg−1 cm−2. Further, a small-scale printable circuit is fabricated using this graphene shows good conductivity of 1.145x103(S/m).

This paper introduces a paper-based closed Au-bipolar electrode (BPE) biosensing system for the rapid and sensitive electrochemiluminescence (ECL) detection of miRNA-155. This microfluidic paper-based sensing platform is formed by wax-printing technology, screen printing method and in-situ Au nanoparticles (NPs) growth to form hydrophilic cells, hydrophobic boundaries, water proof electronic bridge, driving electrode regions and bipolar electrode regions. For rapid and sensitive detection, the cathode of bipolar electrode was modified with the prepared DNA (S1)–AuPd NPs by hybridization chain reaction, in which the target could initiate multiple cycles reaction to load more AuPd NPs which catalyzed H2O2 reduction. In addition, a classical ECL system tris (2,2′-bipyridine) ruthenium (II)- tripropylamine (Ru(bpy)32+/TPrA) exists at the anode of the bipolar electrode. Due to the charge balance between the anode and the cathode of BPE, the ECL signal response of Ru(bpy)32+/TPrA system was enhanced in the reporting cell. The intensity of ECL was quantitatively correlated with the concentration of miRNA-155 in the range of 1 pM–10 μM with the detection limit 0.67 pM. Moreover, this method paves a novel way for highly sensitive detection of miRNA-155 in clinical application.

This work describes the development of a paper-based platform for highly sensitive detection of diclofenac. The quantification of this anti-inflammatory drug is of importance in clinical (e.g. quality and therapeutic control) and environmental (e.g. emerging contaminant determination) areas. The easy-to-handle platform here described consists of a carbon-ink paper-based working electrode and two metallic wires, provided by a gold-plated standard connector, as reference and counter electrodes. The porous paper matrix enables the preconcentration of the sample, decoupling sample and detection solutions. Thus, relatively large sample volumes can be used, which significantly improves the sensitivity of the method. A wide dynamic range of four orders of magnitude, between 0.10 and 100 μM, was obtained for diclofenac determination. Due to the predominance of adsorption at the lowest concentrations, there were two linear concentration ranges: one comprised between 0.10 and 5.0 μM (with a slope of 0.85 μA μM-1) and the other between 5.0 and 100 μM (with a slope of 0.48 μA μM-1). A limit of detection of 70 nM was achieved with this simple device that provided accurate results with an RSD of ca. 5%. The platform was applied for diclofenac quantification in spiked tap water samples. The versatility of this design enabled the fabrication of a multiplexed platform containing eight electrochemical cells that work independently. The low cost, small size and simplicity of the device allow on-site analysis, which is very useful for environmental monitoring., The authors would like to thank the EU and FCT/UEFISCDI/FORMAS for funding, in the frame of the collaborative internationalconsortium REWATERfinanced under the ERA-NET CofundWaterWorks 2015 Call. This ERA-NET is an integral part of the 2016Joint Activities developed by the Water Challenges for a ChangingWorld Joint Programme Initiative (Water JPI). This work was alsosupported by the EU (FEDER funds through COMPETE) and FCT(project FOODnanoHEALTH, Portugal2020, Norte-01-0145-FEDER-000011 and project UID/QUI/50006/2013) and by the SpanishMinistry of Economy and Competitiveness (MINECO, projectCTQ2014-58826-R). Estefanía Costa Rama thanks the Governmentof Principado de Asturias and Marie Curie-Cofund Actions for thepost-doctoral grant“Clarín-Cofund”ACA17-20.

Significance : Cortically implanted microelectrode arrays provide a direct interface with neuronal populations and are used to restore movement capabilities and provide sensory feedback to patients with paralysis or amputation. Penetrating electrodes experience high rates of signal degradation within the first year that limit effectiveness and lead to eventual device failure. Aim : To assess vascular and neuronal changes over time in mice with implanted electrodes and examine the contribution of the brain tissue response to electrode performance. Approach : We used a multimodal approach combining in vivo electrophysiology and subcellular-level optical imaging. Results : At acute timescales, we observed structural damage from the mechanical trauma of electrode insertion, evidenced by severed dendrites in the electrode path and local hypofluorescence. Superficial vessel growth and remodeling occurred within the first few weeks in both electrode-implanted and window-only animals, but the deeper capillary growth evident in window-only animals was suppressed in electrode-implanted animals. After longer implantation periods, there was evidence of degeneration of transected dendrites superficial to the electrode path and localized neuronal cell body loss, along with deep vascular velocity changes near the electrode. Total spike rate (SR) across all animals reached a peak between 3 and 9 months postimplantation, then decreased. The local field potential signal remained relatively constant for up to 6 months, particularly in the high-gamma band, indicating long-term electrode viability and neuronal functioning at further distances from the electrode, but it showed a reduction in some animals at later time points. Most importantly, we found that progressive high-gamma and SR reductions both correlate positively with localized cell loss and decreasing capillary density within 100 μm of the electrode. Conclusions : This multifaceted approach provided a more comprehensive picture of the ongoing biological response at the brain–electrode interface than can be achieved with postmortem histology alone and established a real-time relationship between electrophysiology and tissue damage.

We report a microfluidic paper based analytical device implementing ion concentration polarization (ICP) for rapid pre-concentration of Escherichia coli in water. The fabricated device consists of a paper channel with a Nafion® membrane and in-built micro wire electrodes to supply electric voltage to induce the ICP effect. E. coli cells were stained with SYTO 9 and fluorescence was used as a sensing method. The device achieved high concentration factor up to 2 × 105 within minutes. The effect of total ion concentration, on ICP and fluorescence intensity was studied. The reported device and method are suitable and effective for detection of E. coli during ballast water quality monitoring, coastal water quality monitoring where high salinity water is present.

This paper describes the use of aluminum and zinc as anodic materials for a battery employing nickel (II) oxide (NiO) as cathode. Comparison of both materials resulted in the development of a compact, cost effective, and easy to use primary NiO/Al battery employing an alkaline electrolyte. The system features electrodes composed of powder forms of the active materials on modified paper substrates that are contained in a simple multilayer design utilizing thin laminated plastic materials to provide structure and flexibility to the battery as well as a paper separator. Various concentrations of potassium hydroxide (KOH) electrolyte were examined and maximum performance was observed at 6 M KOH. A maximum current density and power density of 1.94 mA/cm2 and 1 mW/cm2 , respectively was achieved. This user-friendly device was able to produce a maximum capacity of 2.33 mAh/g when 2 mA/g was applied. This work demonstrates the viability of a paper-based battery featuring powder electrodes as a possible power source for microelectronic devices.

A paper-based electrochemical sensor is described that is based on the use of thiol-terminated poly(2-methacryloyloxyethyl phosphorylcholine) (PMPC-SH) that was self-assembled on a gold nanoparticle-modified screen-printed electrode (SPE). The SPE sensor was used for label-free detection of C-reactive protein (CRP). Gold nanoparticles (AuNPs) were first electrodeposited on the SPCE, followed by the self-assembly of PMPC-SH on gold. The electrochemical response of the modified SPE to CRP was measured by differential pulse voltammetry (DPV). If the CRP on the paper device is contacted with Ca (II) ions, the current (measured by using hexacyanoferrate as the electrochemical probe) decreases. The signal drops in the 5 to 5000 ng·mL−1 CRP concentration range, and the lower detection limit (at 3 SD/slope) is 1.6 ng·mL−1. The use of a PMPC-modified surface also reduces the nonspecific adsorption of proteins. The sensor is not interfered by bilirubin, myoglobin and albumin. It was successfully applied to CRP detection in certified human serum. This sensor is applicable as an attractive protocol for an inexpensive, highly sensitive, and disposable material for electrochemical detection of CRP.

A paper-based analytical device (PAD) with an integrated composite electrode for non-enzymatic creatinine sensing was developed. The electrode was produced and optimization was efficiently accomplished using a rapid digital dispensing approach. The electrochemical sensor was fabricated using an HP D300 digital dispenser to deliver a copper oxide and ionic liquid composite onto an electrochemically reduced graphene modified screen-printed carbon electrode (CuO/IL/ERGO/SPCE) on a PAD. The modified electrode was characterized using electrochemical and microscopic techniques. Electrochemical detection of creatinine was performed on the SPCE using amperometry at a constant potential. Under optimized conditions, the paper-based sensor exhibited a linear range of 0.01–2.0 mM (R2 = 0.99) and the limit of detection was 0.22 μM (S/N = 3, IUPAC definition) for creatinine. The simple fabrication process, low cost, and clinically appropriate creatinine sensitivity make this device applicable for point-of-care use.

We report an entirely new class of printed electrical gas sensors that are produced at near “zero cost”. This technology exploits the intrinsic hygroscopic properties of cellulose fibers within paper; although it feels and looks dry, paper contains substantial amount of moisture, adsorbed from the environment, enabling the use of wet chemical methods for sensing without manually adding water to the substrate. The sensors exhibit high sensitivity to water-soluble gases (e.g., lower limit of detection for NH3 < 200 parts-per-billion) with a fast and reversible response. The sensors show comparable or better performance (especially at high relative humidity) than most commercial ammonia sensors at a fraction of their price (

A novel electrochemical glucose sensor was created for a simple but semiquantitative visual screening of specific glucose concentrations in urine. This noninvasive glucose biosensor integrated a disposable, paper-based sensing strip and a simple amplifier circuit with a visual readout. The paper strip consisted of five enzyme-activated electrodes. Each electrode was connected to a specific indicator circuit that triggered a light-emitting diode (LED) when a predefined glucose concentration was reached. The device features (1) low-cost, disposable, paper-based glucose oxidase (GOx)/poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) sensing electrodes, (2) simple signal amplification, and (3) on-site, rapid, and visual detection. The sensor generated reliable, discrete visual responses to determine five glucose levels (1, 2, 3, 4, and higher than 4 mM) in urine in less than 2 min. This innovative approach will provide a simple but powerful glucose sensing paradigm for use in POC diagnostics.

Hemoglobin A1c (HbA1c) is a standard biomarker to measure long-term average glucose concentration for diagnosis and monitoring of diabetes. Various methods have been reported for measuring HbA1c, however, portable and precise determination is still challenging. Herein, a new highly sensitive electrochemical nanobiosensor is developed for the specific determination of HbA1c. A nanocomposite of reduced graphene oxide (rGO) and gold with hierarchical architecture structure was electrochemically deposited on a cheap and flexible graphite sheet (GS) electrode. The nanocomposite increased the surface area, improved the electron transfer on the electrode surface and augmented the signal. It also provided a suitable substrate for linkage of thiolated DNA aptamer as a bioreceptor on the electrode surface by strong covalent bonding. The quantitative label free detection was carried out by differential pulse voltammetry (DPV) in a phosphate-buffered saline (PBS) solution containing redox probe Fe(CN)63−/4-. The detection is based on insulating the surface in presence of HbA1c and decreasing the current, which is directly related to the HbA1c concentration. The nanobiosensor demonstrated high sensitivity of 269.2 μA. cm−2, wide linear range of 1 nM–13.83 μM with a low detection limit of 1 nM. The biosensor was successfully used for measuring HbA1c in blood real sample. Furthermore, it is promising to use it as a part of a point of care device for low-invasive screening and management of diabetes.

This article describes the device design and fabrication of two different configurations (flow-through and stopped-flow) of a sequential fluid delivery platform on a microfluidic paper-based device. The developed device is capable of storing and transporting reagents sequentially to the detection channel without the need for external power. The device comprises two components: an origami folding paper (oPAD) and a movable reagent-stored pad (rPAD). This 3D capillary-driven device eliminates the undesirable procedure of multiple-step reagent manipulation in a complex assay. To demonstrate the scope of this approach, the device is used for electrochemical detection of biological species. Using a flow-through configuration, a self-calibration plot plus real sample analysis using a single buffer introduction are established for ascorbic acid detection. We further broaden the effectiveness of the device to a complex assay using a stopped-flow configuration. Unlike other electrochemical paper-based sensors in which the user is required to cut off the device inlet or rest for the whole channel saturation before measurement, herein a stopped-flow device is carefully designed to exclude the disturbance from the convective mass transport. As a proof of concept, multiple procedures for electrode modification and voltammetric determination of serotonin are illustrated. In addition, the research includes an impedimetric label-free immunosensor for α-fetoprotein using the modified stopped-flow device. The beneficial advantages of simplicity, low sample volume (1 μL), and ability to perform a complex assay qualify this innovative device for use with diverse applications.

Ionogels are semi-solid, ion conductive and mechanically compliant materials that hold promise for flexible, shape-conformable and all-solid-state energy storage devices. However, identifying facile routes for manufacturing ionogels into devices with highly resilient electrode/electrolyte interfaces remains a challenge. Here we present a novel all-in-gel supercapacitor consisting of an ionogel composite electrolyte and bucky gel electrodes processed using a one-step method. Compared with the mechanical properties and ionic conductivities of pure ionogels, our composite ionogels offer enhanced self-recovery (retaining 78% of mechanical robustness after 300 cycles at 60% strain) and a high ionic conductivity of 8.7 mS cm−1, which is attributed to the robust amorphous polymer phase that enables facile permeation of ionic liquids, facilitating effective diffusion of charge carriers. We show that development of a supercapacitor with these gel electrodes and electrolytes significantly improves the interfacial contact between electrodes and electrolyte, yielding an area specific capacitance of 43 mF cm−2 at a current density of 1.0 mA cm−2. Additionally, through this all-in-gel design a supercapacitor can achieve a capacitance between 22–81 mF cm−2 over a wide operating temperature range of −40 °C to 100 °C at a current density of 0.2 mA cm−2.

This work reports a new paper-based sensing platform and its application in a label-free potentiometric immunosensor for Salmonella typhimurium detection based on the blocking surface principle. A paper-based strip electrode was integrated with a filter paper pad which acted as a reservoir of the internal solution. The design offers a convenient platform for antibody immobilization and sampling, proving also that is a simple and affordable methodology to control an ionic flux through a polymer membrane. Two different immunosensing interfaces were assembled on the developed paper-strip electrode. The simplest interface relied on direct conjugation of the antibody to the polymer membrane and the second one resorted to an intermediate layer of a polyamidoamine dendrimer, with an ethylenediamine core from the fourth generation. Electrochemical impedance spectroscopy was used to assess the successive interface modification steps and the resulting analytical performance of both immunosensors was compared. For such, the potential shift derived from the blocking effect of the ionic flux caused by antigen-antibody conjugation was correlated with the logarithm of the Salmonella typhimurium concentration in the sample. In optimized conditions, a limit of detection of 5 cells mL-1 was achieved. As a proof-of-concept, the proposed method was applied to apple juice samples, demonstrating to be a suitable prototype to be used in real scenarios in useful time (, This work received financial support from the European Union and National Funds(FCT, Fundação para a Ciência e Tecnologia) through projects UID/QUI/50006/2019 and Norte-01-0145-FEDER-000011-RL1–QUALIFOOD. N.F.D Silva is grateful to FCT grant SFRH/BD/112414/2015, financed by POPH–QREN–Tipologia 4.1–FormaçãoAvançada,subsidizedbyFSEandMCTES.