Noninvasive Label-Free Detection of Cortisol and Lactate Using Graphene Embedded Screen-Printed Electrode

A sensitive and specific immunosensor for the detection of the hormones cortisol and lactate in human or animal biological fluids, such as sweat and saliva, was devised using the label-free electrochemical chronoamperometric technique. By using these fluids instead of blood,the biosensor becomes noninvasive and is less stressful to the end user, who may be a small child or a farm animal.Electroreduced graphene oxide(e-RGO) was used as a synergistic platform for signal amplification and template for bioconjugation for the sensing mechanism on a screenprinted electrode. The cortisol and lactate antibodies were bioconjugated to the e-RGO using covalent carbodiimide chemistry. Label-free electrochemical chronoamperometric detection was used to analyze the response to the desired biomolecules over the wide detection range. A detection limit of 0.1 ng mL^(-1) for cortisol and 0.1 mM for lactate was established and a correlation between concentration and current was observed. A portable, handheld potentiostat assembled with Bluetooth communication and battery operation enables the developed system for point-of-care applications. A sandwich-like structure containing the sensing mechanisms as a prototype was designed to secure the biosensor to skin and use capillary action to draw sweat or other fluids toward the sensing mechanism. Overall, the immunosensor shows remarkable specificity, sensitivity as well as the noninvasive and point-of-care capabilities and allows the biosensor to be used as a versatile sensing platform in both developed and developing countries.

A sensitive electrochemical detection of metronidazole in synthetic serum and urine samples using low-cost screen-printed electrodes modified with reduced graphene oxide and C60

Monitoring the concentration of antibiotics in body fluids is essential to optimizing the therapy and minimizing the risk of bacteria resistance,which can be made with electrochemical sensors tailored with appropriate materials.In this paper,we report on sensors made with screen-printed electrodes(SPE)coated with fullerene(C60),reduced graphene oxide(rGO)and Nafion(NF)(C60-rGO-NF/SPE)to determine the antibiotic metronidazole(MTZ).Under optimized conditions,the C60-rGO-NF/SPE sensor exhibited a linear response in square wave voltammetry for MTZ concentrations from 2.5×10^(-7) to 34×10^(-6) mol/L,with a detection limit of 2.1×10^(-7) mol/L.This sensor was also capable of detecting MTZ in serum and urine,with recovery between 94%and 100%,which are similar to those of the standard chromatographic method(HPLC-UV).Because the C60-rGO-NF/SPE sensor is amenable to mass production and allows for MTZ determination with simple principles of detection,it fulfills the requirements of therapeutic drug monitoring programs.

Anodic voltammetric determination of gemifloxacin using screen-printed carbon electrode

The electrochemical oxidation behavior and voltammetric assay of gemifloxacin were investigated using differential-pulse and cyclic voltammetry on a screen-printed carbon electrode.The effects of pH,scan rates,and concentration of the drug on the anodic peak current were studied.Voltammograms of gemifloxacin in Tris-HCl buffer（pH 7.0） exhibited a well-defined single oxidation peak.A differential-pulse voltammetric procedure for the quantitation of gemifloxacin has been developed and suitably validated with respect to linearity,limits of detection and quantification,accuracy,precision,specificity,and robustness.The calibration was linear from 0.5 to 10.0 μM,and the limits of detection and quantification were 0.15 and 5.0 μM.Recoveries ranging from 96.26% to 103.64% were obtained.The method was successfully applied to the determination of gemifloxacin in pharmaceutical tablets without any pre-treatment.Excipients present in the tablets did not interfere in the assay.

Amperometric Hydrogen Peroxide Biosensor Based on Horseradish Peroxidase Entrapped in Titania Sol-Gel Film on Screen-Printed Electrode

We report the fabrication of disposable and flexible Screen-Printed Electrodes (SPEs). This new type of screen-printed electrochemical platform consists of Ag nanoparticles (AgNPs) and graphite composite. For this purpose, silver nanoparticles were first synthesized by a chemical reduction method. The morphology and structure of the AgNPs were analyzed using a Scanning Electron Microscope (SEM) and UV-Visible spectroscopy. Graphite was chosen as the working electrode material for the fabrication of a thick-film. The fabrication of a screen-printed hydrogen peroxide biosensor consisting of three electrodes on a polyethylene terephthalate (PET) substrate was performed with a spraying approach (working, counter and reference: enzyme electrode, graphite, pseudo reference: Ag/AgCl). This biosensor was fabricated by immobilizing the peroxidase enzyme (HRP) in a Titania sol-gel membrane which was obtained through a vapor deposition method. The biosensor had electrocatalytic activity in the reduction of H2O2 with linear dependence on H2O2 concentration in the range of 10-5 to 10-3 M;the detection limit was 4.5 × 10-6 M.

Gold Nanoparticles/Thermochromic Composite Film on Screen-Printed Electrodes for Simultaneous Detection of Protein and Temperature

In this study, gold nanoparticles and thermochromic composite films modified screen-printed carbon electrodes (TM-AuNPsSPCEs) were developed as a platform for the simultaneous detection of protein and temperature. The TM-AuNPs composited film had better sensitivity resulting from the gold nanoparticles amplification effect. A phase transition model analysis of TM-AuNPs films found that the TM-AuNPs films had three-phase transition intervals (<45℃, 45℃ to 80℃ and >80℃) which accommodated the temperature requirements for protein denaturation. When used to detect different concentrations of haemoglobin (Hb) solution, the TM-AuNPs modified SPCEs had a better sensitivity in detecting the different concentrations in comparison to TM and AuNP modified SPCEs which showed no clear sensitivity towards the different Hb concentrations. The dual detection and excellent sensitivity show a good application prospect for the study of the TM-AuNPs composite film.

Aptasensor Based on Screen-Printed Carbon Electrodes Modified with CS/AuNPs for Sensitive Detection of Okadaic Acid in Shellfish

Okadaic acid(OA),a small molecule substance derived from shellfish,is one of the most widely distributed marine toxins with acute symptoms of vomiting and diarrhea after accidental ingestion.For this,there is an urgently need for sensitive and reliable methods to detect OA in real shellfish samples.In this study,a simple aptasensor based on screen-printed carbon electrode(SPCE)with modification of chitosan(CS)and gold nanoparticles(Au NPs)was designed for electrochemical determination of OA,and the electrode surface was modified with Au NPs by potential-sweeping electrodeposition,which greatly improved the electrochemical response.The entire detection and characterization process were carried out by cyclic voltammetry(CV)with a linear correlation in the range of 0.01-100 ng/m L and a limit of detection(LOD)of 6.7 pg/m L.Furthermore,recovery rates of 92.3-116%were obtained demonstrating excellent accuracy through the recovery trial of mussel and scallop samples.

Exceeding the limit of plasmonic light trapping in textured screen-printed solar cells using Al nanoparticles and wrinkle-like graphene sheets

The solar cell market is predominantly based on textured screen-printed solar cells.Due to parasitic absorption in nanostructures,using plasmonic processes to obtain an enhancement that exceeds 2.5%of the short-circuit photocurrent density is challenging.In this paper,a 7.2%enhancement in the photocurrent density can be achieved through the integration of plasmonic Al nanoparticles and wrinkle-like graphene sheets.For the first time,we experimentally achieve Al nanoparticle-enhanced solar cells.An innovative thermal evaporation method is proposed to fabricate low-coverage Al nanoparticle arrays on solar cells.Due to the ultraviolet(UV)plasmon resonance of Al nanoparticles,the performance enhancement of the solar cells is significantly greater than that from Ag nanoparticles.Subsequently,we deposit wrinkle-like graphene sheets over the Al nanoparticle-enhanced solar cells.Compared with planar graphene sheets,the bend carbon layer also exhibits a broadband light-trapping effect.Our results exceed the limit of plasmonic light trapping in textured screen-printed silicon solar cells.

Rapid detection of organophosphorus pesticide residue on Prussian blue modified dual-channel screen-printed electrodes combing with portable potentiostat

A novel electrochemical method for the rapid detection of organophosphorus pesticide residues was realized on a dual-channel screen-printed electrode （DSPE） that was integrated with a portable smartphone-controlled potentiostat. The two carbon working channels of DSPE were first modified by electrodepositing of Prussian blue. The channels were then modified with acetylcholinesterase （ACHE） via Nation. The inhibition ratio of AChE was detected by comparing the electrical current of acetylthiocholine （ATCh） that was catalyzed by the enzyme electrodes with （channel 1） and without （channel 2） organophosphorus pesticide. Inhibition ratios were related with the negative logarithm of the organophosphorus pesticide （trichlorfon, oxamyl, and isocarbophos） concentrations at optimum experimental conditions （pH 6.9 of electrolyte, 0.2V working potential, 2.5μL AChE modification amount, and 15 min inhibition time）. The linear equations were 1%=32.301gC＋ 253.3 （R=0.9750） for isocarbophos, I% = 35.991gC＋ 270.1 （R = 0.9668） for chlorpyrifos, and 1% = 33.701gC＋ 250.5 （R = 0.9606） for trichlorfon. The detection limits were calculated as 10-7 g/mL. Given that the inhibition ratios were only related with pesticide concentration and not with pesticide species, the proposed electrodes and electrometer can rapidly detect universal organophosphorus pesticides and assess pesticide pollution.

Graphene oxide/multi-walled carbon nanotubes/gold nanoparticle hybridfunctionalized disposable screen-printed carbon electrode to determine Cd(II)and Pb(II)in soil

Cadmium(Cd)and lead(Pb)in soil or water environment cause the ecological destruction and environmental deterioration when their contents exceed the natural background values.To trace the concentrations of Cd(II)and Pb(II),a sensitive and selective electrode was developed using disposable screen-printed carbon electrode(SPE)immobilized with a composite film of reduced graphene oxide/carboxylation multi-walled carbon nanotubes/gold nanoparticle hybrid(RGO-MWNT-AuNP)throughπ-πbind.This highly conductive nano-composite layer,“RGO-MWNT-AuNP,”was characterized by scanning electron microscopy,UV-visible spectrometer,cyclic voltammetry,and electrochemical impedance spectroscopy.Square wave stripping voltammetry was applied to RGO-MWNT-AuNP/SPE to electroplate bismuth film and monitor the Cd(II)and Pb(II)simultaneously.To obtain high current responses,the detecting parameters were optimized.Under optimized conditions,the current responses showed a linear relationship with the concentrations of Cd(II)and Pb(II)in the range from 1.0 to 80.0μg/L with a lower detection limit of 0.7μg/L and 0.3μg/L(S/N=3),respectively.Finally,the prepared electrode was further employed to detect Cd(II)and Pb(II)in soil samples with good results.

Disposable amperometric biosensors based on xanthine oxidase immobilized in the Prussian blue modified screen-printed three-electrode system

The screen-printed three-electrode system was applied to fabricate a new type of disposable amperometric xanthine oxidase biosensor.Carbon-working,carbon-counter and Ag/AgCl reference electrodes were all manually printed on the polyethylene terephthalate substrate forming the screen-printed three-electrode system by the conventional screen-printing process.As a mediator,Prussian blue could not only catalyze the electrochemical reduction of hydrogen peroxide produced from the enzyme reaction,but also keep the favorable potential around 0 V.The optimum operational conditions,including pH,potential and temperature,were investigated.The sensitivities of xanthine and hypoxanthine detections were 13.83 mA/M and 25.56 mA/M,respectively.A linear relationship was obtained in the concentration range between 0.10μM and 4.98μM for xanthine and between 0.50μM and 3.98μM for hypoxanthine.The small Michaelis-menten constant value of the xanthine oxidase biosensor was calculated to be 3.90 μM.The results indicate that the fabricated xanthine oxidase biosensor is effective and sensitive for the detection of xanthine and hypoxanthine.

A screen-printed, amperometric biosensor for the determination of organophosphorus pesticides in water samples

An amperometric biosensor based on screen-printed electrodes （SPEs） was developed for the determination of organophosphorus pesticides in water samples. The extent of acetylcholinesterase （AChE） deactivation was determined and quantified for pesticide concentrations in water samples. An enzyme immobilization adsorption procedure and polyacrylamide gel matrix polymerization were used for fabrication of the biosensor, with minimal losses in enzyme activity. The optimal conditions for enzyme catalytic reaction on the SPEs surfaces were acetylthiocholine chloride （ATChCl） concentration of 5 mmol/L, pH 7 and reaction time of 4 min. The detection limits for three organophosphorus pesticides （dichlorvos, monocrotophs and parathion） were in the range of 4 to 7 μg/L when an AChE amount of 0.1 U was used for immobilization.

Screen-Printable Functional Nanomaterials for Flexible and Wearable Single-Enzyme-Based Energy-Harvesting and Self-Powered Biosensing Devices

Developing flexible bioelectronics is essential to the realization of artificial intelligence devices and biomedical applications, such as wearables, but their potential is limited by sustainable energy supply. An enzymatic biofuel cell(BFC) is promising for power supply, but its use is limited by the challenges of incorporating multiple enzymes and rigid platforms. This paper shows the first example of screen-printable nanocomposite inks engineered for a single-enzyme-based energy-harvesting device and a self-powered biosensor driven by glucose on bioanode and biocathode. The anode ink is modified with naphthoquinone and multiwalled carbon nanotubes(MWCNTs), whereas the cathode ink is modified with Prussian blue/MWCNT hybrid before immobilizing with glucose oxidase. The flexible bioanode and the biocathode consume glucose. This BFC yields an open circuit voltage of 0.45 V and a maximum power density of 266 μW cm-2. The wearable device coupled with a wireless portable system can convert chemical energy into electric energy and detect glucose in artificial sweat. The self-powered sensor can detect glucose concentrations up to 10 mM. Common interfering substances,including lactate, uric acid, ascorbic acid, and creatinine, have no effect on this self-powered biosensor. Additionally, the device can endure multiple mechanical deformations. New advances in ink development and flexible platforms enable a wide range of applications, including on-body electronics, self-sustainable applications, and smart fabrics.

Flexible planar micro supercapacitor diode

Supercapacitor diode is a novel ion device that performs both supercapacitor energy storage and ion diode rectification functions.However,previously reported devices are limited by their large size and complex processes.In this work,we demonstrate a screen-printed micro supercapacitor diode(MCAPode)that based on the insertion of a finger mode with spinel ZnCo_(2)O_(4) as cathode and activated carbon as anode for the first time,and featuring an excellent area specific capacitance(1.21 mF cm^(-2)at 10 mV s^(-1))and high rectification characteristics(rectification ratioⅠof 11.99 at 40 mV s^(-1)).Taking advantage of the ionic gel electrolyte,which provides excellent stability during repeated flexing and at high temperatures.In addition,MCAPode exhibits excellent electrochemical performance and rectification capability in"AND"and"OR"logic gates.These findings provide practical solutions for future expansion of micro supercapacitor diode applications.

The Influencing Factors of Disposable Acetylcholinesterase Biosensor for in Situ Detection of Organophosphorus Pesticide

An amperometric biosensor based on acetylcholinesterase (ACHE) is assembled by simple adsorption of the AChE on 7,7,8,8-tetracyanoquinodimethane (TCNQ) modified screen-printed electrodes.This biosensor is used to detect the inhibitory effect of organophosphorus pesticides on AChE activity.The detection of organophosphorus pesticides is done with acetylthiocboline chloride (ATCh) as substrate.In order to obtain the optimized response to substrate,the influencing factors of the biosensor are investigated,including temperature,pH,incubation time,substrate concentration and AChE concentration. The measurements were performed after inhibition by immersing the enzyme electrode into the parathion methyl solution. Under the optimized conditions,that is,500 U/ml AChE concentration,pH 7.2,10 min incubation time,2 mmol/L substrate concentration and temperature of 37℃,from 5×10^(-8) mol/L to 5×10^(-5) mol/L is close to linear (regression equation: y(%)=124.055+15.7991gx,R^2=0.99644),which corresponds to 8.7%～56.1% AChE inhibition.With the optimized conditions, the lowest detectable amount of parathion methyl is 13×10^(-9).

Disposable Amperometric Acetylcholinesterase Biosensor for the Detection of Organophosphorus Pesticides

A rapid,simple,disposable and inexpensive acetylcholinesterase (ACHE) amperometric biosensor for the detection of organophosphorus pesticides was developed by simple adsorption of the enzyme on screen-printed electrodes.The biosensor consisted of an Ag/AgCl reference electrode and a graphite working electrode.The mixture of graphite and the 7,7,8,8-tetracyanoquinodimethane (TCNQ) was printed on electrodes.The detection of organophosphorus pesticides was done with acetylthiocholine chloride (ATCh) as substrate.The biosensor was used to detect the inhibitory effect of organophosphorus pesticides on AChE activity.The 1μl of enzyme solution containing 0.1 U AChE and 1% bovine serum albumin (BSA) were simply dropped on the working electrode surface.The biosensor operated at a potential of 300 mV vs. Ag/AgCl in a pH 7.2 0.1 mol/L phosphate buffer and 0.1 mol/L KCl.We obtained a calibration plot of the percentage inhibition versus the logarithm of parathion methyl concentration following an incubation time of 10 mix in parathion methyl solution. The lowest detectable amount of parathion methyl was 0.026 ppm.The amperometric biosensor based on acetylcholinesterase was disposable and low cost (about 1 yuan RMB).

A flow chemiluminescence paper-based microfuidic device for detection of chromium(Ⅲ)in water

In this work,a solely gravity and capillary force-driven flow chemiluminescence(GCF-CL)paper-based microfuidic device has been proved for the first time as a new platforn for inex-pensive,usable,mini mally instrumented dynamic chemiluninescence(CL)detection of chromium(Ⅲ)[Cr(Ⅲ)],where an appropriate angle of inclination between the loading and detection zones on the paper produces a rapid flow of CL prompt solution through the paper charnel.For this study,we use a cost-effective paper device that is manufactured by a simple wax screen-printing method,while the signal generated from the Cr(Ⅲ)-catalyzed oxidation of luminol by H_(2)O_(2) is recorded by a low-cost and luggable CCD camera.A series of GCF-CL affecting factors have been evaluated carefully.At optimal conditions,two linear relationships between GCF-CL intensities and the logarithms of Cr(Ⅲ)concentrations are obtained in the concentration mnges of 0.025-35 mg/L and 50-500 mg/L separately,with the detection limit of 0.0245mg/L for a les than 30s assay,and relative standard deviations(RSDs)of 38%,4.5%and 2.3%for 0.75,5 and 50 mg/L of Cr(Ⅲ)(n=8).The above results indicate that the GCF-CL paper-based microfluidic device possesses a receivable sensitivity,dynamic range,storage stability and reproducibility.Finally,the developed GCF-CL is utilized for Cr(Ⅲ)detection in real water samples.

Bilayered Glass-Ceramics as Sealants for SOFCs

Glass-ceramics are often used as sealants in solid oxide fuel cells (SOFC). But interfacing components, such as ferritic stainless steel and YSZ electrolyte, may vary in their requirements regarding sealing properties, especially in terms of thermal expansion. A bilayered glass-ceramic system was developed to overcome the mismatch in coefficients of thermal expansion (CTE) between ferritic steel and YSZ. Therefore, two different glass-ceramics with slightly different CTEs were developed, one with good bonding characteristics to the ferritic steel and the other to the YSZ electrolyte. Steel and electrolyte components were coated with a layer of their corresponding glass sealant paste and heated up to form a sandwich sample. During the heat treatment of the sealing process, the glasses are crystallized into glass-ceramics. The resulting interface between the two glass-ceramics is of special interest. Cross-sections of the sandwich samples were cut, polished and investigated using SEM. The glass-ceramics show continuous, gap-free layers and excellent bonding to both steel and YSZ. Energy release rates are measured for single and bilayered glass sealants by mechanical testing. The designed bilayered glass-ceramics fulfill the special requirements of ferritic steel and YSZ. They show excellent potential to become a new outstanding sealant for SOFCs.

Self-powered nanofiber-based screen-print triboelectric sensors for respiratory monitoring

Scientific and commercial advances have set high requirements for wearable electronics. However, the power supply, breathability, and mass production of wearable electronics still have many challenges that need to be overcome. In this study, a self-powered nanofiber-based triboelectric sensor （SNTS） was fabricated by batch-scale fabrication technologies using electrospinning and screen-printing for health monitoring via respiratory monitoring. Typically, an arch structural SNTS is assembled by a nanofiber membrane and a Ag nanoparticle electrode. The pile of nanofibers and the conductive network of Ag nanoparticles ensure a gas channel across the whole device. The gas permeability of the SNTS was as high as 6.16 mm/s, which has overwhelming advantages when compared with commonly used wearable devices composed of air-tight cast films. Due to the softness of the nanofiber membrane, the SNTS showed excellent electronic output performance irrespective of whether it was bent, twisted, or folded. The superior properties, such as breathability, skin-friendliness, self-power, and batch fabrication of SNTS offer huge potential for their application in healthcare monitoring and multifunctional intelligent systems.

A potentiometric cobalt-based phosphate sensor based on screen-printing technology

A potentiometric cobalt-based screen-pritning sensor was fabricated by electroplating cobalt on the surface of a screen-printing electrode as the sensitive layer for the determination of dihydrogenphosphate （H2PO4） in wastewater samples. The electrochemical performance of this sensor was fully examined to determine its detection calibration, detection limit, response time, selectivity, and interference with pH, various ions, and dissolved oxygen （DO）. The cobalt-based phosphate sensor showed a phosphate-selective potential response in the range of 10 5mol·L^-1 to 10^-1 mol^-1, yielding a detection limit of 3.16 × 10μmol·L^l and a slope of -37.51 mV·decade＇ in an acidic solution （pH 4.0） of H2PO4-. DO and pH were found to interfere with sensor responses to phosphate. Ultimately, the performance of the sensor was validated for detecting wastewater samples from the Xiaojiahe Waste- water Treatment Plant against the standard speetrophotometric methods for HzPO4 analysis. The discrepancy between the two methods was generally ＋5% （relative standard deviation）. Aside from its high selectivity, sensitivity, and stability, which are comparable with conventional bulk Co-wire sensors, the proposed phosphate sensor presents many other advantages, such as low price, compactness, ease of use, and the possibility of integration with other analytical devices, such as flow injectors.

Design of portable electrochemiluminescence sensing systems for point-of-care-testing applications

Point-of-care testing(POCT)technology is highly desirable for clinical diagnosis,healthcare monitoring,food safety inspection,and environment surveillance,because it enables rapid detection anywhere,anytime,and by anyone.Electrochemiluminescence(ECL)has been widely used in chemo-/bio analysis due to its advantages such as high sensitivity,simplicity,rapidity and easy to control,and is now attracting increasing attention for POCT applications.However,to realize the accurate on-site quantitation,it is still challenging to develop portable devices which can precisely collect,analyze,transmit and display the ECL signals.This review will focus on how to develop a portable ECL device by summarizing recent examples and analyzing their key components part by part.Then the possible solutions to the existing challenges in the development and applications of portable ECL devices are summarized and discussed in detail,followed by offering future perspectives.We attempted to provide an appealing viewpoint to inspire interested researchers to comprehend and explore portable ECL sensing systems for practical applications and even commercialization.