A reusable screen-printed carbon electrode-based aptasensor for the determination of chloramphenicol in food and environment samples.

An electrochemical aptasensor was developed for the determination of chloramphenicol (CAP) in fresh foods and food products. The aptasensor was developed using Prussian blue (PB) and chitosan (CS) film. PB acts as a redox probe for detection and CS acts as a sorption material. The aptamer (Apt) was immobilized on a screen-printed carbon electrode (SPCE) modified with gold nanoparticles (AuNPs). Under optimum conditions, the linearity of the aptasensor was between 1.0 and 6.0 × 106 ng L-1 with a detection limit of 0.65 and a quantification limit of 2.15 ng L-1. The electrode could be regenerated up to 24 times without the use of chemicals. The aptasensor showed good repeatability (RSD <11.2%) and good reproducibility (RSD <7.7%). The proposed method successfully quantified CAP in milk, shrimp pond water and shrimp meat with good accuracy (recovery = 88.0 ± 0.6% to 100 ± 2%). The proposed aptasensor could be especially useful in agriculture to ensure the quality of food and the environment and could be used to determine other antibiotics.

Nano-palladium-decorated bismuth sulfide microspheres on a disposable electrode integrated with smartphone-based electrochemical detection of nitrite in food samples.

Nitrite (NO2-) is widely used as an additive to extend the shelf life of food products. Excessive nitrite intake not only causes blood-related diseases but also has the potential risk of causing cancers. A disposable screen-printed electrode was modified with nano­palladium decorated bismuth sulfide microspheres (nanoPd@Bi2S3MS/SPE), and integrated with a smartphone-interfaced potentiostat to develop a portable, electrochemical nitrite sensor. NanoPd@Bi2S3MS was prepared by the hydrothermal reduction of a Bi2S3MS and Pd2+ dispersion and drop cast on the SPE. The nanoPd@Bi2S3MS/SPE was coupled with a smartphone-controlled portable potentiostat and applied to determine nitrite in food samples. The linear range of the sensor was 0.01-500 µM and the limit of detection was 0.0033 µM. The proposed system showed good repeatability, reproducibility, catalytic stability, and immunity to interferences. The proposed electrode material and a smartphone-based small potentiostat created a simple, portable, fast electrochemical sensing system that accurately measured nitrite in food samples.

A dual-electrode label-free immunosensor based on in situ prepared Au-MoO3-Chi/porous graphene nanoparticles for point-of-care detection of cholangiocarcinoma.

A novel label-free electrochemical immunosensor was prepared for the detection of carbohydrate antigen 19-9 (CA19-9) and carcinoembryonic antigen (CEA) as biomarkers of cholangiocarcinoma (CCA). A nanocomposite of gold nanoparticles, molybdenum trioxide, and chitosan (Au-MoO3-Chi) was layer-by-layer assembled on the porous graphene (PG) modified a dual screen-printed electrode using a self-assembling technique, which increased surface area and conductivity and enhanced the adsorption of immobilized antibodies. The stepwise self-assembling procedure of the modified electrode was further characterized morphologically and functionally. The electroanalytical detection of biomarkers was based on the interaction between the antibody and antigen of each marker via linear sweep voltammetry using ferrocyanide/ferricyanide as an electrochemical redox indicator. Under optimized conditions, the fabricated immunosensor showed linear relationships between current change (ΔI) and antigen concentrations in two ranges: 0.0025-0.1 U mL-1 and 0.1-1.0 U mL-1 for CA19-9, and 0.001-0.01 ng mL-1 and 0.01-1.0 ng mL-1 for CEA. The limits of detection (LOD) were 1.0 mU mL-1 for CA19-9 and 0.5 pg mL-1 for CEA. Limits of quantitation (LOQ) were 3.3 mU mL-1 for CA19-9 and 1.6 pg mL-1 for CEA. The selectivity of the developed immunosensor was tested on mixtures of antigens and was then successfully applied to determine CA19-9 and CEA in human serum samples, producing satisfactory results consistent with the clinical method.

Portable contactless caliper.

This work presents a portable optical meter for noncontact thickness measurement. The device shines a focused laser light on a thin and transparent sample, resulting in an interference between light reflecting from the top and from the bottom surface, and the interfering pattern is recorded by a linear sensor array before data analysis with an Arduino microcontroller. The device produced accurate thickness values from glass cover slips and transparent plastic sheets within a fraction of a second per measurement. Additionally, the sample's refractive index is not required a priori. Therefore, it has a high potential to be of use in real-time quality control in transparent thick-film coating and manufacturing.

A wearable electrode based on copper nanoparticles for rapid determination of paraquat.

The application of copper-based nanoparticles synthesized via green synthesis and their integration with a wearable electrode is reported for designing a flexible catalytic electrode on a glove for onsite electroanalysis of paraquat. A copper precursor and an orange extract from Citrus reticulata are used to synthesize an economical electrocatalytic material for supporting the selective and sensitive detection of paraquat. The electrode yields multidimensional fingerprints due to two redox couples in a square wave voltammogram, corresponding to the presence of paraquat. The developed lab-on-a-finger sensor provides the fast electroanalysis of paraquat within 10 s, covering a wide range from 0.50 to 1000 µM, with a low detection limit down to 0.31 µM and high selectivity. It is also possible to use this sensor at a fast scan rate as high as 6 V s-1 (< 0.5 s for a scan). This wearable glove sensor allows the user to directly touch and analyze samples, such as surfaces of vegetables and fruits, to screen the contamination. It is envisioned that these glove-embedded sensors can be applied to the on-site analysis of food contamination and environments.

Molecularly imprinted polymer dual electrochemical sensor for the one-step determination of albuminuria to creatinine ratio (ACR).

The urinary albumin to creatinine ratio (ACR) is a convenient and accurate biomarker of chronic kidney disease (CKD). An electrochemical sensor for the quantification of ACR was developed based on a dual screen-printed carbon electrode (SPdCE). The SPdCE was modified with carboxylated multiwalled carbon nanotubes (f-MWCNTs) and redox probes of polymethylene blue (PMB) for creatinine and ferrocene (Fc) for albumin. The modified working electrodes were then molecularly imprinted with coated with polymerized poly-o-phenylenediamine (PoPD) to form surfaces that could be separately imprinted with creatinine and albumin template molecules. The seeded polymer layers were polymerized with a second coating of PoPD and the templates were removed to form two different molecularly imprinted polymer (MIP) layers. The dual sensor presented recognition sites for creatinine and albumin on different working electrodes, enabling the measurement of each analyte in one potential scan of square wave voltammetry (SWV). The proposed sensor produced linear ranges of 5.0-100 ng mL-1 and 100-2500 ng mL-1 for creatinine, and 5.0-100 ng mL-1 for albumin. LODs were 1.5 ± 0.2 ng mL-1 and 1.5 ± 0.3 ng mL-1, respectively. The dual MIP sensor was highly selective and stable for seven weeks at room temperature. The ACRs obtained using the proposed sensor compared well (P > 0.05) with the results from immunoturbidimetric and enzymatic methods.

A portable electrochemical immunosensor for ovarian cancer uses hierarchical microporous carbon material from waste coffee grounds.

A simple label-free electrochemical immunosensor for ovarian cancer (OC) detection was developed using a hierarchical microporous carbon material fabricated from waste coffee grounds (WCG). The analysis method exploited near-field communication (NFC) and a smartphone-based potentiostat. Waste coffee grounds were pyrolyzed with potassium hydroxide and used to modify a screen-printed electrode. The modified screen-printed electrode was decorated with gold nanoparticles (AuNPs) to capture a specific antibody. The modification and immobilization processes were characterized by cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). The sensor had an effective dynamic range of 0.5 to 50.0 U mL-1 of cancer antigen 125 (CA125) tumor marker with a correlation coefficient of 0.9995. The limit of detection (LOD) was 0.4 U mL-1. A comparison of the results obtained from human serum analysis with the proposed immunosensor and the results obtained from the clinical method confirmed the accuracy and precision of the proposed immunosensor.

Craft-and-Stick Xurographic Manufacturing of Integrated Microfluidic Electrochemical Sensing Platform.

An innovative modular approach for facile design and construction of flexible microfluidic biosensor platforms based on a dry manufacturing "craft-and-stick" approach is developed. The design and fabrication of the flexible graphene paper electrode (GPE) unit and polyethylene tetraphthalate sheet (PET)6/adhesive fluidic unit are completed by an economic and generic xurographic craft approach. The GPE widths and the microfluidic channels can be constructed down to 300 µm and 200 µm, respectively. Both units were assembled by simple double-sided adhesive tapes into a microfluidic integrated GPE (MF-iGPE) that are flexible, thin (<0.5 mm), and lightweight (0.4 g). We further functionalized the iGPE with Prussian blue and glucose oxidase for the fabrication of MF-iGPE glucose biosensors. With a closed-channel PET fluidic pattern, the MF-iGPE glucose biosensors were packaged and sealed to protect the integrated device from moisture for storage and could easily open with scissors for sample loading. Our glucose biosensors showed 2 linear dynamic regions of 0.05-1.0 and 1.0-5.5 mmol L-1 glucose. The MF-iGPE showed good reproducibility for glucose detection (RSD < 6.1%, n = 6) and required only 10 µL of the analyte. This modular craft-and-stick manufacturing approach could potentially further develop along the concept of paper-crafted model assembly kits suitable for low-resource laboratories or classroom settings.

One-step electrodeposition of poly(o-phenylenediamine)-Zn composite on plaswood propeller as an extraction device for polycyclic aromatic hydrocarbons in coffee.

Coffee beans can be contaminated during roasting by polycyclic aromatic hydrocarbons (PAHs), some of which have been classified as carcinogens. An extraction device for PAHs in coffee drinks was designed with six compact DC motors rotating six sorbents. The sorbents were plaswood propellers modified by one-step electrodeposition of a poly(ortho-phenylenediamine) and Zn composite (PoPD-Zn). Benzo(a)anthracene (BaA), chrysene (Chry), benzo(b)fluoranthene (BbF), and benzo(a)pyrene (BaP) were chosen as representative PAHs. Scanning electron micrographs of the PoPD-Zn showed a porous structure. The extracted PAHs were quantified by gas chromatography coupled with a flame ionization detector. Detected concentrations of PAHs in coffee drink samples were as follows: BaA 1.4 ± 0.4 to 16.5 ± 0.8 µg L-1; Chry 0.5 ± 0.2 to 2.1 ± 0.5 µg L-1; BbF 2.2 ± 0.6 µg L-1; and BaP 6.2 ± 1.0 µg L-1. Good recoveries ranging from 82.7 ± 1.9% to 99.0 ± 0.5% were obtained.

A polypyrrole-cotton pad sorbent as micro-solid phase extractor enclosed in tea bag envelope for determination of synthetic antioxidants in non-alcoholic beverage products.

A polypyrrole (PPy)-cotton pad sorbent enclosed in tea bag envelope was developed and used in micro-solid phase extraction (µ-SPE) for the determination of butylated hydroxyanisole (BHA) and butylated hydroxytoluene (BHT). After extraction, the extract was qualified and quantified by a gas chromatograph equipped with a flame ionization detector (GC-FID). Parameters influencing this developed method and the efficiency of µ-SPE were studied and optimized. Under the optimal conditions, the developed method provided good linearity in a concentration range of 0.100-100 µg L-1 for BHA and 0.050-50 µg L-1 for BHT, respectively. The limits of detection were 39.27 ± 0.52 ng L-1 for BHA and 16.96 ± 0.17 ng L-1 for BHT. Satisfactory relative recoveries of BHA and BHT were achieved in the range from 86.8 ± 1.9 to 117.1 ± 2.3% with acceptable relative standard deviation (RSD) below 8.1%. Good reproducibility was obtained with RSDs < 3.1%, for n = 6. The developed adsorbent is easy to operate, low cost, eco-friendly, reusable, with high extraction efficiency, and was successfully applied in the simultaneous synthetic antioxidant determination of non-alcoholic beverage samples.

Novel biosensor platform for glucose monitoring via smartphone based on battery-less NFC potentiostat.

Near-field communication (NFC) was used to control a portable glucose biosensor for diabetes diagnosis. The system comprised a smartphone and an NFC potentiostat connected to a screen-printed carbon electrode (SPCE) modified with Prussian blue-graphene ink and functionalized with gold nanoparticles-embedded poly (3,4ethylene dioxythiophene):polysulfonic acid coated with glucose oxidase (GOx-AuNPs-PEDOT:PSS/PB-G). GOx catalyzed the glucose redox reaction while the conductivity and sensitivity of the AuNPs-PEDOT:PSS composite enhanced electron transfer to the PB-G, which was used as a mediator. The fabrication process was characterized by scanning electron microscopy (SEM) with energy dispersibe x-ray analysis (EDX). The platform was electrochemically characterized by electrical impedance spectroscopy (EIS) and cyclic voltammetry (CV). The NFC biosensing device was then applied to quantify glucose in human blood serum by amperometry. The linear concentration range and detection limit for glucose were 0.5-500 µM and 0.15 µM, respectively. The accuracy of the device was good and results were in agreement with the results obtained from the standard hospital method. This NFC glucose sensing device can be a simple, sensitive, selective and portable platform for medical diagnosis.

Disposable label-free electrochemical immunosensor based on prussian blue nanocubes for four breast cancer tumor markers.

A compact and low-cost multi-electrode array (MEA) is presented, comprising four working electrodes with shared reference and auxiliary electrodes. Prussian blue was electrodeposited on the MEA using chronoamperometry with a positive potential of 0.3 V. Prussian blue nanocubes (PBNCs) were formed, which were observed using scanning electron microscopy. The precision of the four working electrodes was demonstrated using ferric/ferro cyanide (RSD <5.8%). The surface roughness of the working electrodes of the fabricated MEA was investigated by atomic force microscopy and compared with that of a commercial MEA. The PBNCs were the platform for a label-free immunosensor that detected four breast cancer tumor markers (CEA, CA125, CA153, and CA199) using specific antibodies. The processes of antibody immobilization were investigated using cyclic voltammetry and electrochemical impedance spectroscopy. The immunosensor was evaluated using real human serum samples, yielding acceptable recoveries (95.1-104.1%, RSD < 3.9) for the four tumor markers. These findings confirmed that our label-free immunosensor based on PBNCs could be a promising device for point-of-care testing and could pave the way for the establishment of new platforms for the screening of various breast cancer tumor markers.

A wireless smartphone-based "tap-and-detect" formaldehyde sensor with disposable nano-palladium grafted laser-induced graphene (nanoPd@LIG) electrodes.

We developed a fully integrated smart sensing device for on-site testing of food to detect trace formaldehyde (FA). A nano-palladium grafted laser-induced graphene (nanoPd@LIG) composite was synthesized by one-step laser irradiation of a Pd2+-chitosan-polyimide precursor. The composite was synthesized in the form of a three-electrode sensor on a polymer substrate. The electrochemical properties and morphology of the fabricated composite were characterized and the electrochemical kinetics of FA oxidation at the nanoPd@LIG electrode were investigated. The nanoPd@LIG electrode was combined with a smart electrochemical sensing (SES) device to determine FA electrochemically. The proposed SES device uses near field communication (NFC) to receive power and transfer data between a smartphone interface and a battery-free sensor. The proposed FA sensor exhibited a linear detection range from 0.01 to 4.0 mM, a limit of detection of 6.4 µM, good reproducibility (RSDs between 2.0 and 10.1%) and good anti-interference properties for FA detection. The proposed system was used to detect FA in real food samples and the results correlated well with the results from a commercial potentiostat and a spectrophotometric analysis.

Electrochemical sensor based on molecularly imprinted polymer cryogel and multiwalled carbon nanotubes for direct insulin detection.

Insulin is the polypeptide hormone that regulates blood glucose levels. It is used as an indicator of both types of diabetes. An electrochemical insulin sensor was developed using a gold electrode modified with carboxylated multiwalled carbon nanotubes (f-MWCNTs) and molecularly imprinted polymer (MIP) cryogel. The MIP provided specific recognition sites for insulin, while the macropores of the cryogel promoted the mass transfer of insulin to the recognition sites. The f-MWCNTs increased the effective surface area and conductivity of the sensor and also reduced the potential required to oxidize insulin. Insulin oxidation was directly measured in a flow system using square wave voltammetry. This MIP cryogel/f-MWCNTs sensor provided a linear range of 0.050-1.40 pM with a very low limit of detection (LOD) of 33 fM. The sensor exhibited high selectivity and long-term stability over 10 weeks of dry storage at room temperature. The results of insulin determination in human serum using the sensor compared well with the results of the Elecsys insulin assay. The developed MIP sensor offers a promising alternative for the diagnosis and treatment of diabetes.

Waste polystyrene foam-derived sorbent for determining bisphenol-A from canned beverages.

Polystyrene-based products are widely used in industrial and daily activities, but their subsequent disposal can negatively affect the environment. This work focuses on reducing polystyrene waste into useful material. A waste-derived polystyrene sorbent (WDPS) was fabricated and successfully applied to determine bisphenol-A in canned beverages. High-performance liquid chromatography with a diode-array detection (HPLC-DAD) was applied to quantify bisphenol-A. Good linearity at a concentration range of 2.5-50 µg L-1 was achieved. The limit of detection was 0.93 ± 0.02 µg L-1. Good precision (RSDs < 1.6 %, 4 concentrations, n = 6) in spiked coconut juice samples were obtained. The contamination of BPA in canned beverage samples were found in the range of 6.3 ± 0.2 µg L-1 to 27.0 ± 1.0 µg L-1 with recoveries in the range of 70.4 ± 1.6 % to 82.4 ± 0.4 %. This proposed method also offers reduced polystyrene waste, reuse as a sorbent, and recycling after use.

Flow Injection Amperometric Measurement of Formalin in Seafood.

Formalin is illegally used as an antibacterial and a preservative in seafood products. It is extremely important for public health reasons to be able to simply, rapidly, and accurately detect formalin in fresh seafood. In this work, we developed a flow injection amperometric (FI-Amp) formalin sensor based on a glassy carbon electrode modified with a composite of palladium particles and carbon microspheres (PdPs-CMs/GCE). The CMs were decorated with PdPs via an electroless deposition method. The surface morphology of the CMs and the PdPs-CMs composite was characterized by scanning electron microscopy/energy dispersive X-ray spectroscopy (SEM/EDX). The electrochemical behavior and measurement of formalin at the PdPs-CMs/GCE was evaluated by cyclic voltammetry and amperometry. The modified electrode demonstrated good electrocatalytic performance for the oxidation of formalin. The synthesis method and FI-Amp operating conditions were optimized. Under the optimal conditions, the developed sensor showed a linear range of 0.025 to 15.00 mmol L-1 and a detection limit of 8 µmol L-1. Repeatability (RSD < 4.1%, n = 30), reproducibility (RSD = 0.25%, n = 5), stability (RSD = 3.2%, n = 80), and selectivity were good. The fabricated sensor achieved recoveries of formalin in seafood between 96 ± 1 to 105 ± 3 (n = 3).

A stir bar sorptive extraction device coupled with a gas chromatography flame ionization detector for the determination of abused prescription drugs in lean cocktail samples.

A lean cocktail is a mixed drink for the non-medical use of prescription medications that has emerged in recent years as a drug of abuse and is related to drug-facilitated crimes. The determination of active ingredients in a lean cocktail is necessary for forensic investigations. This work presents an in-house developed stir bar sorptive extraction (SBSE) device with an XAD-2 adsorbent followed by analysis using GC-FID for the extraction and determination of the five main abused prescription drugs (diphenhydramine, tramadol, chlorpheniramine, dextromethorphan and promethazine) in lean cocktail samples. Under optimized conditions, the developed method provided linearity for 1.0-250 µg mL-1 of each of the five abused prescription drugs. The limits of detection and limits of quantitation were in the respective ranges of 0.25-0.5 µg mL-1 and 1.0-1.5 µg mL-1. The percentage of extraction was 85.0-94.9%. The intra-day and inter-day precisions were 1.2-14.4% RSD and 1.4-15.8% RSD, respectively. Good relative recoveries in the range of 86.7-110.3% and 88.5-107.9% were obtained when the proposed method was applied for extraction and analysis of abused prescription drugs in five lean cocktail samples. The developed method can be a useful tool for measuring the levels of abused prescription drugs in a lean cocktail and the data could also be used as evidence in a forensic investigation.

Portable device for dual detection of fluorescence and absorbance for biosensing or chemical sensing applications.

Early detection is key to prevent health problems and could be performed by biosensors and chemical sensors. However, a lot of them still need bulky benchtop equipment. This work presents a portable device for measuring fluorescence and light absorption that can be used with optical biosensors or chemical sensors. It uses a small laser diode as a light source and three filter-mounted photodiodes as detectors, all of which are inexpensive, customizable and widely available commercially. The results from our device show good correlation with that from commercial instruments. Therefore, it could be beneficial for early or on-site detection.

A Fabrication of Multichannel Graphite Electrode Using Low-Cost Stencil-Printing Technique.

Multichannel graphite electrodes (MGrEs) have been designed and fabricated in this study. A template was cut from an adhesive plastic sheet using a desktop cutting device. The template was placed on a polypropylene substrate, and carbon graphite ink was applied with a squeegee to the template. The size of the auxiliary electrode (AE) as well as the location of the reference electrode (RE) of MGrEs design were investigated. Scanning electron microscopy was used to determine the thickness of the ink on the four working electrodes (WEs), which was 21.9 ± 1.8 µm. Cyclic voltammetry with a redox probe solution was used to assess the precision of the four WEs. The intra-electrode repeatability and inter-electrode reproducibility of the MGrEs production were satisfied by low RSD (<6%). Therefore, the MGrEs is reliable and capable of detecting four replicates of the target analyte in a single analysis. The electrochemical performance of four WEs was investigated and compared to one WE. The sensitivity of the MGrEs was comparable to the sensitivity of a single WE. The MGrEs' potential applications were investigated by analyzing the nitrite in milk and tap water samples (recoveries values of 97.6 ± 0.4 to 110 ± 2%).

Fluorescent cysteine probe based on a signal amplification unit, a catalyzed hairpin assembly reaction and Förster resonance energy transfer.

This work developed a sensitive DNA-based fluorescent probe comprising a cysteine binding unit and a signal amplification unit based on a catalyzed hairpin assembly (CHA) reaction. The cysteine binding unit comprises a homodimer of single-stranded DNA (ssDNA) rich in cytosine and held together by silver ions. In the presence of cysteine, the homodimer is disintegrated because of cysteine-silver binding that liberates the ssDNA, which drives the CHA reaction in the signal amplification unit. Förster resonance energy transfer (FRET) was used to report the generation of the amplified double-stranded DNA (dsDNA) product. Under the optimal conditions, the probe provided a good linearity (100-1200 nM), a good detection limit (47.8 ± 2.7 nM) and quantification limit (159.3 ± 5.3 nM), and a good sensitivity (1.900 ± 0.045µM-1). The probe was then used to detect cysteine in nine real food supplement samples. All results provided good recoveries that are acceptable by the AOAC, indicating that it has potential for practical applications.