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.

Electropolymerization of poly(phenol red) on laser-induced graphene electrode enhanced adsorption of zinc for electrochemical detection.

We present a highly sensitive and selective electrode of laser-induced graphene modified with poly(phenol red) (P(PhR)@LIG) for measuring zinc nutrition in rice grains using square wave anodic stripping voltammetry (SWASV). The physicochemical properties of P(PhR)@LIG were investigated with scanning electron microscopy (SEM), energy-dispersive X-ray (EDX), Fourier infrared spectroscopy (FT-IR) and Raman spectroscopy. The modified electrode demonstrated an amplified anodic stripping response of Zn2+ due to the electropolymerization of P(PhR), which enhanced analyte adsorption during the accumulation step of SWASV. Under optimized parameters, the developed sensor provided a linear range from 30 to 3000 µg L-1 with a detection limit of 14.5 µg L-1. The proposed electrode demonstrated good reproducibility and good anti-interference properties. The sensor detected zinc nutrition in rice grain samples with good accuracy and the results were consistent with the standard ICP-OES method.

A novel 3D-printed portable electroplating device enhances latent fingerprints on metal substrates.

This work introduces a 3D-printed portable electroplating device for the visualization of latent fingerprints (LFPs) on metallic substrates. An electroplating solution of Ag+-Cu2+ in a deep eutectic solvent (DES) is used. The electroplating is performed by two electrodes equivalent to an anode (+) and a cathode (-). The cathode is connected to the metal surface with the magnetic or alligator clip for carrying the LFP. The anode is connected to cotton dipped in the electroplating solution. The device was optimized in terms of the electroplating solution composition, and electroplating potential, current, and time. The device produced images with good resolution, revealing LFP ridges in minute detail of more than 12 points. The device also exhibited good repeatability and images were assessed against guidelines from the Centre for Applied Science and Technology (CAST) and the International Fingerprint Research Group (IFRG). The developed device could be applied to visualize LFPs in forensic investigations.

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.

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.

Nanocoral-like Polyaniline-Modified Graphene-Based Electrochemical Paper-Based Analytical Device for a Portable Electrochemical Sensor for Xylazine Detection.

A portable electrochemical device for xylazine detection is presented for the first time. An electrochemical paper-based analytical device (ePAD) was integrated with a smartphone. The fabrication of the ePAD involved wax printing, low-tack transfer tape, and cutting and screen-printing techniques. Graphene ink was coated on the substrate and modified with nanocoral-like polyaniline, providing an electron transfer medium with a larger effective surface area that promoted charge transfer. The conductive ink on the ePAD presented a thickness of 25.0 ± 0.9 µm for an effective surface area of 0.374 cm2. This sensor was then tested directly on xylazine using differential pulse voltammetry. Two linear responses were obtained: from 0.2 to 5 µg mL-1 and from 5 to 100 µg mL-1. The detection limit was 0.06 µg mL-1. Reproducibility was tested on 10 preparations. The relative standard deviation was less than 5%. The applicability of the sensor was evaluated with beverage samples spiked with trace xylazine. Recoveries ranged from 84 ± 4 to 105 ± 2%. The developed sensor demonstrated excellent accuracy in the detection of trace xylazine. It would be possible to develop the portable system to detect various illicit drugs to aid forensic investigations.

Facile fabrication of a flexible laser induced gold nanoparticle/chitosan/ porous graphene electrode for uric acid detection.

We developed a simple, inexpensive, environmentally friendly one-step fabrication of a flexible laser induced graphene-chitosan-gold nanoparticles (LIG-CS-AuNPs) electrode. The fabrication was based on a laser treatment of polyimide (PI) film coated with CS solution containing gold ions (Au (III)). The AuNPs decorating the induced 3D graphene composite were uniformly distributed. The electrode exhibited good electrical conductivity and excellent electrocatalytic activity toward the oxidation of UA. To enable on-site monitoring of uric acid (UA) in blood serum by differential pulse adsorptive stripping voltammetry (DPAdSV), the electrode was coupled to a portable potentiostat connected to a cellphone to control and monitor analysis. The affecting parameters of DPAdSV were optimized. Under the optimal conditions for UA determination, the limit of detection of the developed sensor was 0.33 µmol L-1 and the limit of quantification 1.10 µmol L-1. Two linear ranges were produced: 1.0-30 µmol L-1 and 30-100 µmol L-1. The sensor was highly sensitive and demonstrated excellent reproducibility and selectivity, determining UA in blood serum with recoveries between 86.6 ± 0.6 and 94.7 ± 0.4%. The analysis results were in agreement with those of the hospital standard enzymatic method.

Discrimination of dopamine by an electrode modified with negatively charged manganese dioxide nanoparticles decorated on a poly(3,4 ethylenedioxythiophene)/reduced graphene oxide composite.

A unique nanocomposite was fabricated using negatively charged manganese dioxide nanoparticles, poly (3,4-ethylenedioxythiophene) and reduced graphene oxide (MnO2/PEDOT/rGO). The nanocomposite was deposited on a glassy carbon electrode (GCE) functionalized with amino groups. The modified GCE was used to electrochemically detect dopamine (DA). The surface morphology, charge effect and electrochemical behaviours of the modified GCE were characterized by scanning electron microscopy, energy dispersive X-ray analysis (EDX), cyclic voltammetry and electrochemical impedance spectroscopy, respectively. The MnO2/PEDOT/rGO/GCE exhibited excellent performance towards DA sensing with a linear range between 0.05 and 135 µM with a lowest detection limit of 30 nM (S/N = 3). Selectivity towards DA was high in the presence of high concentrations of the typical interferences ascorbic acid and uric acid. The stability and reproducibility of the electrode were good. The sensor accurately determined DA in human serum. The synergic effect of the multiple components of the fabricated nanocomposite were critical to the good DA sensing performance. rGO provided a conductive backbone, PEDOT directed the uniform growth of MnO2 and adsorbed DA via pi-pi and electrostatic interaction, while the negatively charged MnO2 provided adsorption and catalytic sites for protonated DA. This work produced a promising biosensor that sensitively and selectively detected DA.

A portable electrochemical sensor for detection of the veterinary drug xylazine in beverage samples.

A portable electrochemical sensor was developed to determine xylazine in spiked beverages by adsorptive stripping voltammetry (AdSV). The sensor was based on a graphene nanoplatelets-modified screen-printed carbon electrode (GNPs/SPCE). The electrochemical behavior of xylazine at the GNPs/SPCE was an adsorption-controlled irreversible oxidation reaction. The loading of graphene nanoplatelets (GNPs) on the modified SPCE, electrolyte pH, and AdSV accumulation potential and time were optimized. Under optimal conditions, the GNPs/SPCE provided high sensitivity, linear ranges of 0.4-6.0 mg L-1 (r = 0.997) and 6.0-80.0 mg L-1 (r = 0.998) with a detection limit of 0.1 mg L-1 and a quantitation limit of 0.4 mg L-1. Repeatability was good. The accuracy of the proposed sensor was investigated by spiking six beverage samples at 1.0, 5.0, and 10.0 mg L-1. The recoveries from this method ranged from 80.8 ± 0.2-108.1 ± 0.3 %, indicating the good accuracy of the developed sensor. This portable electrochemical sensor can be used to screen for xylazine in beverage samples as evidence in cases of sexual assault or robbery.

Electrochemical Sensor for Methamphetamine Detection Using Laser-Induced Porous Graphene Electrode.

A 3D porous graphene structure was directly induced by CO2 laser from the surface of Kapton tape (carbon source) supported by polyethylene terephthalate (PET) laminating film. A highly flexible laser-induced porous graphene (LI-PGr) electrode was then fabricated via a facile one-step method without reagent and solvent in a procedure that required no stencil mask. The method makes pattern design easy, and production cost-effective and scalable. We investigated the performance of the LI-PGr electrode for the detection of methamphetamine (MA) on household surfaces and in biological fluids. The material properties and morphology of LI-PGr were analysed by scanning electron microscopy (SEM), energy dispersive x-ray (EDX) and Raman spectroscopy. The LI-PGr electrode was used as the detector in a portable electrochemical sensor, which exhibited a linear range from 1.00 to 30.0 µg mL-1 and a detection limit of 0.31 µg mL-1. Reproducibility was good (relative standard deviation of 2.50% at 10.0 µg mL-1; n = 10) and anti-interference was excellent. The sensor showed good precision and successfully determined MA on household surfaces and in saliva samples.

Subnanomolar detection of promethazine abuse using a gold nanoparticle-graphene nanoplatelet-modified electrode.

A simple, sensitive, and effective adsorptive stripping voltammetric sensor for the detection of trace-level promethazine was created based on a gold nanoparticle-graphene nanoplatelet-modified glassy carbon electrode (AuNP-GrNP/GCE). AuNP-GrNP nanocomposites were synthesized using an electroless deposition process, and the morphology was characterized using UV-vis spectroscopy, Fourier transform infrared spectroscopy, field emission scanning electron microscopy, and energy-dispersive X-ray spectroscopy. The electrochemical behavior and detection of promethazine at the AuNP-GrNP/GCE were investigated utilizing cyclic voltammetry and adsorptive stripping voltammetry. The AuNP-GrNP/GCE showed outstanding synergistic electrochemical activity for promethazine oxidation, a highly active surface area, great adsorptivity, and outstanding catalytic properties. The electrolyte pH, amount of AuNP-GrNP nanocomposite, preconcentration potential (vs. Ag/AgCl), and time were optimized to obtain a high performance electrochemical sensor. Under optimal conditions, the proposed sensor displayed two linear concentration ranges from 1.0 nmol L-1 to 1.0 µmol L-1 and from 1.0 to 10 µmol L-1. The limits of detection and quantitation were 0.40 and 1.4 nmol L-1, respectively. This sensor displayed high sensitivity, a capability for rapid analysis, and excellent repeatability and reproducibility. The developed sensor was effective and practical for promethazine detection in biological fluids and forensic samples, and the obtained results exhibited excellent agreement with the results obtained using the method described in the British Pharmacopoeia. Graphical abstract.

Porous palladium-poly(3,4-ethylenedioxythiophene)-coated carbon microspheres/graphene nanoplatelet-modified electrode for flow-based-amperometric hydrazine sensor.

A highly stable flow-injection amperometric hydrazine sensor was developed based on a glassy carbon electrode modified with palladium-poly(3,4-ethylene dioxythiophene) coated on carbon microspheres/graphene nanoplatelets (Pd-PEDOT@CM/GNP/GCE). The Pd-PEDOT@CM/GNP composite was characterized by scanning electron microscopy and energy-dispersive x-ray analysis (SEM/EDX). The modified GCE was electrochemically characterized using cyclic voltammetry and chronoamperometry. The electrocatalytic activity of the Pd-PEDOT@CM/GNP/GCE toward hydrazine oxidation was significantly better than the activity of a bare GCE, a CM/GCE, a GNP/GCE, a Pd-PEDOT/GCE, and a Pd-PEDOT@CM/GCE. The sensor operated best at a low working potential of + 0.10 V (vs. Ag/AgCl). Under optimal conditions, sensitivity toward hydrazine detection and operational stability (601 injections/one electrode preparation) were excellent. The response was linear from 1.0 to 100 µmol L-1 and from 100 to 5000 µmol L-1 with a detection limit of 0.28 ± 0.02 µmol L-1 and high sensitivity of 0.200 µA µM-1 cm-2. The sensor showed good repeatability (relative standard deviation (RSD) < 1.4%, n = 15), reproducibility (RSD < 2.7%, n = 6), and anti-interference characteristics toward hydrazine detection. The feasibility of the electrochemical sensor was proved by the successful determination of hydrazine in water samples, and the results were in good agreement with those obtained from spectrophotometric analysis. Graphical abstract.

Bio-PEDOT: Modulating Carboxyl Moieties in Poly(3,4-ethylenedioxythiophene) for Enzyme-Coupled Bioelectronic Interfaces.

Modulation of chemical functional groups on conducting polymers (CPs) provides an effective way to tailor the physicochemical properties and electrochemical performance of CPs, as well as serves as a functional interface for stable integration of CPs with biomolecules for organic bioelectronics (OBEs). Herein, we introduced a facile approach to modulate the carboxylate functional groups on the PEDOT interface through a systematic evaluation on the effect of a series of carboxylate-containing molecules as counterion dopant integrated into the PEDOT backbone, including acetate as monocarboxylate (mono-COO-), malate as dicarboxylate (di-COO-), citrate as tricarboxylate (tri-COO-), and poly(acrylamide-co-acrylate) as polycarboxylate (poly-COO-) bearing different amounts of molecular carboxylate moieties to create tunable PEDOT:COO- interfaces with improved polymerization efficiency. We demonstrated the modulation of PEDOT:COO- interfaces with various granulated morphologies from 0.33 to 0.11 µm, tunable surface carboxylate densities from 0.56 to 3.6 µM cm-2, and with improved electrochemical kinetics and cycling stability. We further demonstrated the effective and stable coupling of an enzyme model lactate dehydrogenase (LDH) with the optimized PEDOT:poly-COO- interface via simple covalent chemistry to develop biofunctionalized PEDOT (Bio-PEDOT) as a lactate biosensor. The biosensing mechanism is driven by a sequential bioelectrochemical signal transduction between the bio-organic LDH and organic PEDOT toward the concept of all-polymer-based OBEs with a high sensitivity of 8.38 µA mM-1 cm-2 and good reproducibility. Moreover, we utilized the LDH-PEDOT biosensor for the detection of lactate in spiked serum samples with a high recovery value of 91-96% and relatively small RSD in the range of 2.1-3.1%. Our findings provide a new insight into the design and optimization of functional CPs, leading to the development of new OBEs for sensing, biosensing, bioengineering, and biofuel cell applications.

Adsorption and determination of sibutramine in illegal slimming product using porous graphene ink-modified electrode.

This work presents a new material, i.e., a porous graphene ink to modify on the GCE surface (PGr-ink/GCE) to improve sensitivity by increasing the surface area of the electrode for the electrochemical determination of sibutramine. The surface characterization and electrochemical adsorption behavior of the PGr-ink/GCE toward sibutramine were investigated using scanning electron microscopy (SEM), cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), ATR-FTIR spectroscopy and square wave adsorptive stripping voltammetry (SWAdSV). The PGr-ink/GCE exhibited a distinctive anodic response towards sibutramine using SWAdSV in BR buffer (pH 8.00) with a sensitivity 4 times higher than the bare GCE. Under the optimum conditions, the modified electrode showed good electrochemical adsorption and detection of sibutramine by the SWAdSV method with two ranges of linear concentration from 0.015 to 10.0 µg mL-1 and 10-50 µg mL-1. The limit of detection and quantitation were 5 ng mL-1 and 15 ng mL-1, respectively. Over a short analysis time (180 s), the sensor exhibited high sensitivity (10.9 µAµg-1mLcm-2), good reproducibility (RSD <3.4% n = 6), repeatability (RSD between 1.8 and 9.8% (n = 15)), excellent anti-interference properties and was successfully applied for the quantification of sibutramine in different brands of illegal slimming products with good recoveries (93 ± 4-104 ± 1%). The developed electrochemical sibutramine sensor is suitable for application in detecting illegal components in slimming products.