Search Results (42)

Molecular sensor systems, e.g., implantables and wearables, provide extensive health-related monitoring. Glucose sensor systems have historically prevailed in wearable bioanalysis applications due to their continuous and reliable glucose monitoring, a feat not yet accomplished for other biomarkers. However, the advancement of reagentless detection methodologies may facilitate the creation of molecular sensor systems for multiple analytes. Improving the sensitivity and selectivity of molecular sensor systems is also crucial for biomarker detection under intricate physiological circumstances. The term multidomain molecular sensor systems is utilized to refer, in general, to both biological and chemical sensor systems. This review examines methodologies for enhancing signal amplification, improving selectivity, and facilitating reagentless detection in multidomain molecular sensor devices. The review also analyzes the fundamental components of multidomain molecular sensor systems, including substrate materials, bodily fluids, power, and decision-making units. The review article further investigates how extensive data gathered from multidomain molecular sensor systems, in conjunction with current data processing algorithms, facilitate biomarker detection for precision medicine. Full article

Enzyme-based biosensors commonly utilize the drop-casting method for their surface modification. However, the drawbacks of this technique, such as low reproducibility, coffee ring effects, and challenges in mass production, hinder its application. To overcome these limitations, we propose a novel surface functionalization strategy of enzyme crosslinking via inkjet printing for reagentless enzyme-based biosensors. This method includes printing three functional layers onto a screen-printed electrode: the enzyme layer, crosslinking layer, and protective layer. Nanomaterials and substrates are preloaded together during our inkjet printing. Inkjet-printed electrodes feature a uniform enzyme deposition, ensuring high reproducibility and superior electrochemical performance compared to traditional drop-casted ones. The resultant biosensors display high sensitivity, as well as a broad linear response in the physiological range of the serum phosphate. This enzyme crosslinking method has the potential to extend into various enzyme-based biosensors through altering functional layer components. Full article

Two types of low-cost reagentless electrochemical glucose biosensors based on graphite rod (GR) electrodes were developed. The electrodes modified with electrochemically synthesized platinum nanostructures (PtNS), 1,10-phenanthroline-5,6-dione (PD), glucose oxidase (GOx) without and with a polypyrrole (Ppy) layer—(i) GR/PtNS/PD/GOx and (ii) GR/PtNS/PD/GOx/Ppy, respectively, were prepared and tested. Glucose biosensors based on GR/PtNS/PD/GOx and GR/PtNS/PD/GOx/Ppy electrodes were characterized by the sensitivity of 10.1 and 5.31 μA/(mM cm²), linear range (LR) up to 16.5 and 39.0 mM, limit of detection (LOD) of 0.198 and 0.561 mM, good reproducibility, and storage stability. The developed glucose biosensors based on GR/PtNS/PD/GOx/Ppy electrodes showed exceptional resistance to interfering compounds and proved to be highly efficient for the determination of glucose levels in blood serum. Full article

Spectral point-of-care technology is reagentless with minimal sampling (<10 μL) and can be performed in real-time. White blood cells are non-dominant in blood and in spectral information, suffering significant interferences from dominant constituents such as red blood cells, hemoglobin and billirubin. White blood cells of a bigger size can account for 0.5% to 22.5% of blood spectra information. Knowledge expansion was performed using data augmentation through the hybridization of 94 real-world blood samples into 300 synthetic data samples. Synthetic data samples are representative of real-world data, expanding the detailed spectral information through sample hybridization, allowing us to unscramble the spectral white blood cell information from spectra, with correlations of 0.7975 to 0.8397 and a mean absolute error of 32.25% to 34.13%; furthermore, we achieved a diagnostic efficiency between 83% and 100% inside the reference interval (5.5 to 19.5 × 10${}^9$ cell/L), and 85.11% for cases with extreme high white blood cell counts. At the covariance mode level, white blood cells are quantified using orthogonal information on red blood cells, maximizing sensitivity and specificity towards white blood cells, and avoiding the use of non-specific natural correlations present in the dataset; thus, the specifity of white blood cells spectral information is increased. The presented research is a step towards high-specificity, reagentless, miniaturized spectral point-of-care hematology technology for Veterinary Medicine. Full article

Quenchbody (Q-body) is a unique, reagentless, fluorescent antibody whose fluorescent intensity increases in an antigen-concentration-dependent manner. Q-body-based homogeneous immunoassay is superior to conventional immunoassays as it does not require multiple immobilization, reaction, and washing steps. In fact, simply mixing the Q-body and the sample containing the antigen enables the detection of the target antigen. To date, various Q-bodies have been developed to detect biomarkers of interest, including haptens, peptides, proteins, and cells. This review sought to describe the principle of Q-body-based immunoassay and the use of Q-body for various immunoassays. In particular, the Q-bodies were classified from a structural perspective to provide useful information for designing Q-bodies with an appropriate objective. Full article

Precise blood glucose detection plays a crucial role in diagnosing and medicating diabetes, in addition to aiding diabetic patients in effectively managing their condition. In this research, a first-generation reagentless amperometric glucose biosensor was developed by combining the graphite rod (GR) electrode modification by gold nanostructures (AuNS) and Prussian blue (PB) with glucose oxidase (GOx)—an enzyme that can oxidize glucose and produce H₂O₂. Firstly, AuNS was electrochemically deposited on the GR electrode (AuNS/GR), and then PB was electrochemically synthesized on the AuNS/GR electrode (PB/AuNS/GR). Finally, GOx was immobilized over the PB/AuNS nanocomposite with the assistance of Nafion (Nf) (Nf-GOx/PB/AuNS/GR). An application of PB in the design of a glucose biosensor enables an easy electrochemical reduction and, thus, the determination of the H₂O₂ produced during the GOx-catalyzed oxidation of glucose in the sample at a low operation potential of −0.05 V vs. Ag/AgCl/KCl_{3 mol L}⁻¹. In addition, AuNS increased the electrochemically active surface area, improved the GOx immobilization and ensured a higher analytical signal. The developed glucose biosensor based on the Nf-GOx/PB/AuNS/GR electrode exhibited a wide linear range, from 0.025 to 1 mmol L⁻¹ of glucose, with a 0.0088 mmol L⁻¹ limit of detection, good repeatability and high selectivity over electroactive interfering substances. The developed biosensor is convenient for the determination of glucose in the physiological environment. Full article

Reagentless electrochemical glucose biosensors were developed and investigated. A graphite rod (GR) electrode modified with electrochemically synthesized dendritic gold nanostructures (DGNs) and redox mediators (Med) such as ferrocenecarboxylic acid (FCA), 1,10-phenathroline-5,6-dione (PD), N,N,N′,N′-tetramethylbenzidine (TMB) or tetrathiafulvalene (TTF) in combination with glucose oxidase (GOx) (GR/DGNs/FCA/GOx, GR/DGNs/PD/GOx, GR/DGNs/TMB/GOx, or GR/DGNs/TTF/GOx) were developed and electrochemically investigated. A biosensor based on threefold-layer-by-layer-deposited PD and GOx (GR/DGNs/(PD/GOx)₃) was found to be the most suitable for the determination of glucose. To improve the performance of the developed biosensor, the surface of the GR/DGNs/(PD/GOx)₃ electrode was modified with polypyrrole (Ppy) for 5 h. A glucose biosensor based on a GR/DGNs/(PD/GOx)₃/Ppy_{(5 h)} electrode was characterized using a wide linear dynamic range of up to 39.0 mmol L⁻¹ of glucose, sensitivity of 3.03 µA mM⁻¹ cm⁻², limit of detection of 0.683 mmol L⁻¹, and repeatability of 9.03% for a 29.4 mmol L⁻¹ glucose concentration. The Ppy-based glucose biosensor was characterized by a good storage stability (τ_1/2 = 9.0 days). Additionally, the performance of the developed biosensor in blood serum was investigated. Full article

Electrochemical impedance spectroscopy (EIS) is a sensitive analytical method for surface and bulk properties. Classical EIS and derived electrochemical capacitance spectroscopy (ECS) with a redox couple are label-free approaches for biosensor development, but doubts arise regarding interpretability when a redox couple is employed (redox EIS) due to interactions between electroactive probes and interfacial charges or forced potential. Here, we demonstrated redoxless ECS for directly determining surfactant adsorption on screen-printed carbon electrodes (SPCEs), validated through a simulation of equivalent circuits and the electrochemistry of electronic dummy cells. Redoxless ECS provides excellent capacitance plot loci for quantifying the interfacial permittivity of di-electric layers on electrode surfaces. Redoxless ECS was compared with redox EIS/ECS, revealing a favorable discrimination of interfacial capacitances under both low and high SDS coverage on SPCEs and demonstrating potential for probeless (reagentless) sensing. Furthermore, the proposed method was applied in an electrolyte without a redox couple and bare electrodes, obtaining a high performance for the adsorption of surfactants Tween-20, Triton-X100, sodium dodecyl sulfate, and tetrapropylammonium bromide. This approach offers a simple and straightforward means for a semi-quantitative evaluation of small molecule interactions with electrode surfaces. Our proposed approach may serve as a starting point for future probeless (reagentless) and label-free biosensors based on electrochemistry, eliminating disturbance with surface charge properties and minimizing forced potential bias by avoiding redox couples. An unambiguous and quantitative determination of physicochemical properties of biochemically recognizable layers will be relevant for biosensor development. Full article

The development of simple and probe-integrated aptamer sensors for the electrochemical detection of tumor biomarkers is of great significance for the diagnosis of tumors and evaluation of prognosis. In this work, a probe-integrated aptamer sensor is demonstrated based on the stable confinement of an electrochemical probe in a bipolar nanochannel film, which can realize the reagentless electrochemical detection of the tumor biomarker carcinoembryonic antigen (CEA). To realize the stable immobilization of a large amount of the cationic electrochemical probe methylene blue (MB), a two-layer silica nanochannel array (SNF) with asymmetric charge was grown on the supporting electrode from bipolar SNF (bp-SNF). The inner SNF is negatively charged (n-SNF), and the outer-layer SNF is positively charged (p-SNF). The dual electrostatic interaction including the electrostatic adsorption from n-SNF and the electrostatic repulsion from p-SNF achieve the stable confinement of MB in bp-SNF. The recognitive interface is fabricated by the covalent immobilization of the CEA aptamer on the outer surface of bp-SNF, followed by the blocking of non-specific binding sites. Owing to the stable and abundant immobilized probes and highly specific aptamer interface, the developed aptamer sensor enables the sensitive detection of CEA in the range of 1 pg/mL to 1 μg/mL with a low limit of detection (LOD, 0.22 pg/mL, S/N = 3). Owing to the high selectivity and stability of the developed biosensor, reagentless electrochemical detection of CEA in serum was realized. Full article

Laser scribing is a technique that converts carbon-rich precursors into 3D-graphene nanomaterial via direct, single-step, and maskless laser writing in environmental conditions and using a scalable approach. It allows simple, fast, and reagentless production of a promising material with outstanding physicochemical features to create novel electrochemical sensors and biosensors. This review addresses different strategies for fabricating laser-scribed graphene (LSG) devices and their association with nanomaterials, polymers, and biological molecules. We provide an overview of their applications in environmental and health monitoring, food safety, and clinical diagnosis. The advantages of their integration with machine learning models to achieve low bias and enhance accuracy for data analysis is also addressed. Finally, in this review our insights into current challenges and perspectives for LSG electrochemical sensors are presented. Full article

Electrodialysis (ED) is an attractive method of tartrate stabilization of wine due to its rapidity and reagentlessness. At the same time, fouling of ion-exchange membranes by the components of wine materials is still an unsolved problem. The effect of ethanol, polyphenols (mainly anthocyanins and proanthocyanidins) and saccharides (fructose) on the fouling of aliphatic ion-exchange membranes CJMA-6 and CJMC-5 (manufactured by Hefei Chemjoy Polymer Materials Co. Ltd., Hefei, China) was analyzed using model solutions. It was shown that the mechanism and consequences of fouling are different in the absence of an electric field and during electrodialysis. In particular, a layer of colloidal particles is deposited on the surface of the CJMA-6 anion-exchange membrane in underlimiting current modes. Its thickness increases with increasing current density, apparently due to the implementation of a trap mechanism involving tartaric acid anions, as well as protons, which are products of water splitting and “acid dissociation”. A successful attempt was made to clean CJMA-6 in operando by pumping a water-alcohol solution of KCl through the desalination compartment and changing electric field direction. It has been established that such a cleaning process suppresses the subsequent biofouling of ion-exchange membranes. In addition, selective recovery of polyphenols with high antioxidant activity is possible. Full article

Soil tests for plant-available phosphorus (P) are suggested to provide offsite P analysis required to monitor P fertilizer application and reduce P losses to downstream water. However, procedural and cost limitations of current soil phosphate tests have restricted their widespread use and have made them accessible only in laboratories. This study proposes a novel paper-based reagentless electrochemical soil phosphate sensor to extract and detect soil phosphate using an inexpensive and simple approach. In this test, concentrated Mehlich-3 and molybdate ions were impregnated in filter paper, which served as the phosphate extraction and reaction zone, and was followed by electrochemical detection using cyclic voltammetry signals. Soil samples from 22 sampling sites were used to validate this method against inductively coupled plasma optical emission spectroscopy (ICP) soil phosphate tests. Regression and correlation analyses showed a significant relationship between phosphate determinations by ICP and the proposed method, delivering a correlation coefficient, r, of 0.98 and a correlation slope of 1.02. The proposed approach provided a fast, portable, low-cost, accessible, reliable, and single-step test to extract and detect phosphate simultaneously with minimum waste (0.5 mL per sample), which made phosphate characterization possible in the field. Full article

Bisphenol A (BPA) is widely used in the manufacture of polycarbonate and epoxy-resin-based products, and BPA contamination often happens in a variety of types of environment and food stuffs. BPA can cause many harmful effects to health due to its high toxicity. The rapid detection of BPA is of great significance in environmental monitoring and food safety. Nucleic acid aptamers show advantages in biosensors due to good chemical stability, the ease of labeling functional groups, and target binding that induces conformation change. Here, we performed a thorough characterization of the binding performance of one 60-nt anti-BPA DNA aptamer with isothermal titration calorimetry (ITC). We found the crucial region of the aptamer sequence for affinity binding with BPA, and the aptamer was able to be truncated to 29-nt DNA without losing affinity. We then developed a simple reagent-less electrochemical aptamer-based sensor for rapid BPA detection with this engineered aptamer. The truncated aptamer with a redox tag methylene blue (MB) was immobilized on a gold electrode. BPA-binding induced the conformation change of the MB-labeled aptamer, moving the MB close to the electrode surface and causing a significant current increase in MB in square wave voltammetry (SWV). Under optimized conditions, we achieved the quantitative detection of BPA with a detection limit of BPA at 0.1 μM. This sensor showed quick response to BPA and could be regenerated by washing with deionized water. This sensor was selective, and it allowed detecting BPA in complex samples, showing its potential in practice. This study will help in further applications of the aptamers of BPA. Full article