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1.
Mikrochim Acta ; 191(6): 362, 2024 Jun 01.
Article En | MEDLINE | ID: mdl-38822867

Rapid and accurate in situ determination of dopamine is of great significance in the study of neurological diseases. In this work, poly (3,4-ethylenedioxythiophene): poly (styrenesulfonic acid) (PEDOT: PSS)/graphene oxide (GO) fibers were fabricated by an effective method based on microfluidic wet spinning technology. The composite microfibers with stratified and dense arrangement were continuously prepared by injecting PEDOT: PSS and GO dispersion solutions into a microfluidic chip. PEDOT: PSS/GO fiber microelectrodes with high electrochemical activity and enhanced electrochemical oxidation activity of dopamine were constructed by controlling the structure composition of the microfibers with varying flow rate. The fabricated fiber microelectrode had a low detection limit (4.56 nM) and wide detection range (0.01-8.0 µM) for dopamine detection with excellent stability, repeatability, and reproducibility. In addition, the PEDOT: PSS/GO fiber microelectrode prepared was successfully used for the detection of dopamine in human serum and PC12 cells. The strategy for the fabrication of multi-component fiber microelectrodes is a new and effective approach for monitoring the intercellular neurotransmitter dopamine and has high potential as an implantable neural microelectrode.


Dopamine , Graphite , Microelectrodes , Polystyrenes , PC12 Cells , Dopamine/blood , Humans , Rats , Animals , Polystyrenes/chemistry , Graphite/chemistry , Limit of Detection , Electrochemical Techniques/methods , Electrochemical Techniques/instrumentation , Microfluidic Analytical Techniques/instrumentation , Microfluidic Analytical Techniques/methods , Bridged Bicyclo Compounds, Heterocyclic/chemistry , Thiophenes/chemistry , Lab-On-A-Chip Devices , Polymers
2.
Mikrochim Acta ; 191(6): 361, 2024 Jun 01.
Article En | MEDLINE | ID: mdl-38822891

A one-shot CO2 laser-based strategy to generate conductive reduced graphene oxide (rGO) decorated with nanoceria (nCe) is proposed. The 2D/0D rGO-nCe films, integrated as catalytic sensing layers in paper-based sensors, were employed for on-site monitoring of indoor fogging treatments against Listeria monocytogenes (Lm), a ubiquitous pathogenic bacterium. The rGO-nCe laser-assisted synthesis was optimized to preserve the rGO film morphological and electron-transfer features and simultaneously integrate catalytic nCe. The films were characterized by microscopical (SEM), spectroscopical (EDX, Raman, and FTIR), and electrochemical techniques. The most performing film was integrated into a nitrocellulose substrate, and the complete sensor was assembled via a combination of xurography and stencil printing. The rGO-nCe sensor's catalytic activity was proved toward the detection of H2O2, obtaining sensitive determination (LOD = 0.3 µM) and an extended linear range (0.5-1500 µM). Eventually, the rGO-nCe sensor was challenged for the real-time continuous monitoring of hydrogen peroxide aerosol during no-touch fogging treatment conducted following the EU's recommendation for biocidal product use. Treatment effectiveness was proved toward three Lm strains characterized by different origins, i.e., type strain ATCC 7644, clinical strain 338, and food strain 641/6II. The sensor allows for discrimination and quantification treatments at different environmental biocidal amounts and fogging times, and correlates with the microbiological inhibition, promoting the proposed sensor as a useful tool to modulate and monitor no-touch treatments.


Disinfection , Graphite , Hydrogen Peroxide , Lasers , Listeria monocytogenes , Paper , Graphite/chemistry , Hydrogen Peroxide/chemistry , Listeria monocytogenes/drug effects , Listeria monocytogenes/isolation & purification , Disinfection/methods , Cerium/chemistry , Limit of Detection , Electrochemical Techniques/methods , Electrochemical Techniques/instrumentation , Catalysis
3.
Carbohydr Polym ; 339: 122232, 2024 Sep 01.
Article En | MEDLINE | ID: mdl-38823905

In this study, new types of hybrid double-network (DN) hydrogels composed of polyvinyl alcohol (PVA), chitosan (CH), and sodium alginate (SA) are introduced, with the hypothesis that this combination and incorporating multi-walled carbon nanotubes (MWCNTs) and graphene nanoplatelets (GNPs) will enhance osteogenetic differentiation and the structural and mechanical properties of scaffolds for bone tissue engineering applications. Initially, the impact of varying mass ratios of the PVA/CH/SA mixture on mechanical properties, swelling ratio, and degradability was examined. Based on this investigation, a mass ratio of 4:6:6 was determined to be optimal. At this ratio, the hydrogel demonstrated a Young's modulus of 47.5 ± 5 kPa, a swelling ratio of 680 ± 6 % after 3 h, and a degradation rate of 46.5 ± 5 % after 40 days. In the next phase, following the determination of the optimal mass ratio, CNTs and GNPs were incorporated into the 4:6:6 composite resulting in a significant enhancement in the electrical conductivity and stiffness of the scaffolds. The introduction of CNTs led to a notable increase of 36 % in the viability of MG63 osteoblast cells. Additionally, the inhibition zone test revealed that GNPs and CNTs increased the diameter of the inhibition zone by 49.6 % and 52.6 %, respectively.


Alginates , Bone Regeneration , Chitosan , Hydrogels , Polyvinyl Alcohol , Tissue Engineering , Tissue Scaffolds , Chitosan/chemistry , Alginates/chemistry , Alginates/pharmacology , Polyvinyl Alcohol/chemistry , Tissue Scaffolds/chemistry , Humans , Bone Regeneration/drug effects , Hydrogels/chemistry , Hydrogels/pharmacology , Tissue Engineering/methods , Nanotubes, Carbon/chemistry , Osteoblasts/drug effects , Osteoblasts/cytology , Graphite/chemistry , Graphite/pharmacology , Biomimetic Materials/chemistry , Biomimetic Materials/pharmacology , Cell Survival/drug effects , Cell Line
4.
Anal Chim Acta ; 1310: 342716, 2024 Jun 29.
Article En | MEDLINE | ID: mdl-38811135

BACKGROUND: Assembling framework nucleic acid (FNA) nanoarchitectures and tuning luminescent quantum dots (QDs) for fluorescence assays represent a versatile strategy in analytical territory. Rationally, FNA constructs could offer a preferential orientation to efficiently recognize the target and improve detection sensitivity, meanwhile, regulating size-dependent multicolor emissions of QDs in one analytical setting for ratiometric fluorescence assay would greatly simplify operation procedures. Nonetheless, such FNA/QDs-based ratiometric fluorescence nanoprobes remain rarely explored. RESULTS: We designed a sensitive and signal amplification-free fluorescence aptasensor for lead ions (Pb2+) that potentially cause extensive contamination to environment, cosmetic, food and pharmaceuticals. Red and green emission CdTe quantum dots (rQDs and gQDs) were facilely prepared. Moreover, silica nanosphere encapsulating rQDs served as quantitative internal reference and scaffold to anchor a predesigned FNA and DNA sandwich containing Pb2+ binding aptamer and gQD modified DNA signal reporter. On binding of Pb2+, the gQD-DNA signal reporter was set free, resulting in fluorescence quenching at graphene oxide (GO) interface. Owing to the rigid structure of FNA, the fluorescence signal reporter orderly arranged at the silica nanosphere could sensitively respond to Pb2+ stimulation. The dose-dependent fluorescence signal-off mode enabled ratiometric analysis of Pb2+ without cumbersome signal amplification. Linear relationship was established between fluorescence intensity ratio (I555/I720) and Pb2+ concentration from 10 nM to 2 µM, with detection limit of 1.7 nM (0.43 ppb), well addressing the need for Pb2+ routine monitoring. The designed nanoprobe was applied to detection of Pb2+ in soil, cosmetic, milk, drug, and serum samples, with the sensitivity comparable to conventional ICP-MS technique. SIGNIFICANCE: Given the programmable design of FNA and efficient recognition of target, flexible tuning of QDs emission, and signal amplification-free strategy, the present fluorescence nanoprobe could be a technical criterion for other heavy metal ions detection in a straightforward manner.


DNA , Graphite , Lead , Nanospheres , Quantum Dots , Silicon Dioxide , Spectrometry, Fluorescence , Quantum Dots/chemistry , Lead/analysis , Lead/chemistry , Graphite/chemistry , Silicon Dioxide/chemistry , Nanospheres/chemistry , DNA/chemistry , Cadmium Compounds/chemistry , Limit of Detection , Tellurium/chemistry , Aptamers, Nucleotide/chemistry , Fluorescence , Biosensing Techniques/methods
5.
Mikrochim Acta ; 191(6): 356, 2024 05 29.
Article En | MEDLINE | ID: mdl-38811412

Charged antimicrobial peptides can be used for direct potentiometric biosensing, but have never been explored. We report here a galvanostatically-controlled potentiometric sensor for antimicrobial peptide-based biosensing. Solid-state pulsed galvanostatic sensors that showed excellent stability under continuous galvanostatic polarization were prepared by utilizing reduced graphene oxide/poly (3,4-ethylenedioxythiophene): poly (4-styrenesulfonate) (rGO/PEDOT: PSS) as a solid contact. More importantly, the chronopotentiometric sensor can be made sensitive to antimicrobial peptides with intrinsic charge on demand via a current pulse. In this study, a positively charged antimicrobial peptide that can bind to Staphylococcus aureus with high affinity and good selectivity was designed as a model. Two arginine residues with positive charges were linked to the C-terminal of the peptide sequence to increase its potentiometric responses on the electrode. The bacteria binding-induced charge or charge density change of the antimicrobial peptide enables the direct chronopotentiometric detection of the target. Under the optimized conditions, the concentration of Staphylococcus aureus can be determined in the linear range 10-1.0 × 105 CFU mL-1 with a detection limit of 10 CFU mL-1. It is anticipated that such a chronopotentiometric sensing platform is readily adaptable to detect other bacteria by choosing the peptides.


Biosensing Techniques , Graphite , Potentiometry , Staphylococcus aureus , Biosensing Techniques/methods , Graphite/chemistry , Potentiometry/methods , Antimicrobial Peptides/chemistry , Antimicrobial Peptides/pharmacology , Limit of Detection , Polymers/chemistry , Bridged Bicyclo Compounds, Heterocyclic/chemistry , Bridged Bicyclo Compounds, Heterocyclic/pharmacology , Electrodes
6.
Environ Sci Pollut Res Int ; 31(23): 34607-34621, 2024 May.
Article En | MEDLINE | ID: mdl-38705925

A series of ZnO decorated reduced graphene oxide (rGO) (ZnrGOx) with different doping ratios were synthesized by the alkaline hydrothermal method using graphene oxide (GO) and Zn(NO3)2·6H2O as precursors, and subsequently used for the adsorption study of Cr(VI) in water. The morphology, crystalline phase structure, and surface elemental properties of ZnrGOx composites were revealed by XRD, SEM, BET, FT-IR, and XPS characterizations. The results showed that ZnO nanoparticles can be clearly seen on the surface of layered rGO. Meanwhile, as the doping rate increased, the C = C double bonds were broken and more carboxylic acid groups formed in ZnrGOx. In addition, the ZnrGO0.1 composite had the most excellent adsorption performance and good stability, and reusability. The adsorption removal rate of Cr(VI) can reach 99%, and the maximum adsorption amount of Cr(VI) was 68.9655 mg/g in 3 h. The isothermal and kinetic model simulations showed that Cr(VI) adsorption on ZnrGO0.1 composite is a chemical adsorption process, spontaneous and endothermic. Based on the concentrations of different valence states of Cr in the solid and liquid phases, 40% of Cr(VI) was reduced to Cr(III) on the surface of ZnrGO0.1 composite. Moreover, the adsorption-reduction mechanisms of Cr(VI) on ZnrGO0.1 composite were further elucidated. The ZnrGO0.1 composite manifested great potential as an efficient adsorbent for Cr(VI) removal.


Chromium , Graphite , Water Pollutants, Chemical , Zinc Oxide , Zinc Oxide/chemistry , Adsorption , Graphite/chemistry , Chromium/chemistry , Water Pollutants, Chemical/chemistry , Kinetics , Water Purification/methods
7.
Mikrochim Acta ; 191(6): 301, 2024 05 06.
Article En | MEDLINE | ID: mdl-38709350

In the era of wearable electronic devices, which are quite popular nowadays, our research is focused on flexible as well as stretchable strain sensors, which are gaining humongous popularity because of recent advances in nanocomposites and their microstructures. Sensors that are stretchable and flexible based on graphene can be a prospective 'gateway' over the considerable biomedical speciality. The scientific community still faces a great problem in developing versatile and user-friendly graphene-based wearable strain sensors that satisfy the prerequisites of susceptible, ample range of sensing, and recoverable structural deformations. In this paper, we report the fabrication, development, detailed experimental analysis and electronic interfacing of a robust but simple PDMS/graphene/PDMS (PGP) multilayer strain sensor by drop casting conductive graphene ink as the sensing material onto a PDMS substrate. Electrochemical exfoliation of graphite leads to the production of abundant, fast and economical graphene. The PGP sensor selective to strain has a broad strain range of ⁓60%, with a maximum gauge factor of 850, detection of human physiological motion and personalized health monitoring, and the versatility to detect stretching with great sensitivity, recovery and repeatability. Additionally, recoverable structural deformation is demonstrated by the PGP strain sensors, and the sensor response is quite rapid for various ranges of frequency disturbances. The structural designation of graphene's overlap and crack structure is responsible for the resistance variations that give rise to the remarkable strain detection properties of this sensor. The comprehensive detection of resistance change resulting from different human body joints and physiological movements demonstrates that the PGP strain sensor is an effective choice for advanced biomedical and therapeutic electronic device utility.


Dimethylpolysiloxanes , Graphite , Wearable Electronic Devices , Graphite/chemistry , Humans , Dimethylpolysiloxanes/chemistry , Movement
8.
Luminescence ; 39(5): e4758, 2024 May.
Article En | MEDLINE | ID: mdl-38712530

The ability of heterogeneous photocatalysis to effectively remove organic pollutants from wastewater has shown great promise as a tool for environmental remediation. Pure zinc ferrites (ZnFe2O4) and magnesium-doped zinc ferrites (Mg@ZnFe2O4) with variable percentages of Mg (0.5, 1, 3, 5, 7, and 9 mol%) were synthesized via hydrothermal route and their photocatalytic activity was checked against methylene blue (MB) taken as a model dye. FTIR, XPS, BET, PL, XRD, TEM, and UV-Vis spectroscopy were used for the identification and morphological characterization of the prepared nanoparticles (NPs) and nanocomposites (NCs). The 7% Mg@ZnFe2O4 NPs demonstrated excellent degradation against MB under sunlight. The 7% Mg@ZnFe2O4 NPs were integrated with diverse contents (10, 50, 30, and 70 wt.%) of S@g-C3N4 to develop NCs with better activity. When the NCs were tested to degrade MB dye, it was revealed that the 7%Mg@ZnFe2O4/S@g-C3N4 NCs were more effective at utilizing solar energy than the other NPs and NCs. The synergistic effect of the interface formed between Mg@ZnFe2O4 and S@g-C3N4 was primarily responsible for the boosted photocatalytic capability of the NCs. The fabricated NCs may function as an effective new photocatalyst to remove organic dyes from wastewater.


Ferric Compounds , Methylene Blue , Nitrogen Compounds , Solar Energy , Water Pollutants, Chemical , Zinc , Catalysis , Water Pollutants, Chemical/chemistry , Ferric Compounds/chemistry , Methylene Blue/chemistry , Zinc/chemistry , Magnesium/chemistry , Photolysis , Photochemical Processes , Coloring Agents/chemistry , Nanocomposites/chemistry , Graphite/chemistry , Wastewater/chemistry , Nitriles/chemistry
9.
Mikrochim Acta ; 191(6): 322, 2024 05 10.
Article En | MEDLINE | ID: mdl-38730044

The first electrochemical sensor application in the literature is described for the sensitive and selective determination of the selective Janus kinase (JAK)-1 inhibitor abrocitinib (ABR). ABR is approved by the U.S. Food and Drug Administration (FDA) for the treatment of atopic dermatitis. The molecularly imprinted polymer (MIP)-based sensor was designed to incorporate zinc nanoflower (ZnNFs)-graphene oxide (GO) conjugate (ZnNFs@GO), synthesized from the root methanolic extract (RME) of the species Alkanna cappadocica Boiss. et Bal. to improve the porosity and effective surface area of the glassy carbon electrode (GCE). Furthermore, the MIP structure was prepared using ABR as a template molecule, 4-aminobenzoic acid (4-ABA) as a functional monomer, and other additional components. Scanning electron microscopy (SEM), X-ray diffraction (XRD), and Fourier transform infrared spectroscopy (FTIR) were used to characterize the surface and structure of the synthesized nanomaterial and MIP-based surface. Among the electrochemical methods, cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) were preferred for detailed electrochemical characterization, and differential pulse voltammetry (DPV) was preferred for all other electrochemical measurements using 5.0 mM [Fe(CN)6]3-/4- solution as the redox probe. The MIP-based sensor, which was the result of a detailed optimization phase, gave a linear response in the 1.0 × 10-13 - 1.0 × 10-12 M range in standard solution and serum sample. The obtained limit of detection (LOD) and limit of quantification (LOQ) values and recovery studies demonstrated the sensitivity, accuracy, and applicability of the sensor. Selectivity, the most important feature of the MIP-based sensor, was verified by imprinting factor calculations using ibrutinib, ruxolitinib, tofacitinib, zonisamide, and acetazolamide.


Electrochemical Techniques , Limit of Detection , Molecularly Imprinted Polymers , Zinc , Molecularly Imprinted Polymers/chemistry , Electrochemical Techniques/methods , Electrochemical Techniques/instrumentation , Zinc/chemistry , Graphite/chemistry , Humans , Aminoimidazole Carboxamide/analogs & derivatives , Aminoimidazole Carboxamide/analysis , Aminoimidazole Carboxamide/blood , Aminoimidazole Carboxamide/chemistry , Nanostructures/chemistry , Electrodes
10.
Molecules ; 29(9)2024 Apr 24.
Article En | MEDLINE | ID: mdl-38731427

Dopamine (DA) and uric acid (UA) are essential for many physiological processes in the human body. Abnormal levels of DA and UA can lead to multiple diseases, such as Parkinson's disease and gout. In this work, a three-dimensional reduced graphene oxide-MXene (3D rGO-Ti3C2) composite electrode was prepared using a simple one-step hydrothermal reduction process, which could separate the oxidation potentials of DA and UA, enabling the simultaneous detection of DA and UA. The 3D rGO-Ti3C2 electrode exhibited excellent electrocatalytic activity towards both DA and UA. In 0.01 M PBS solution, the linear range of DA was 0.5-500 µM with a sensitivity of 0.74 µA·µM-1·cm-2 and a detection limit of 0.056 µM (S/N = 3), while the linear range of UA was 0.5-60 µM and 80-450 µM, with sensitivity of 2.96 and 0.81 µA·µM-1·cm-2, respectively, and a detection limit of 0.086 µM (S/N = 3). In 10% fetal bovine serum (FBS) solution, the linear range of DA was 0.5-500 µM with a sensitivity of 0.41 µA·µM-1·cm-2 and a detection limit of 0.091 µM (S/N = 3). The linear range of UA was 2-500 µM with a sensitivity of 0.11 µA·µM-1·cm-2 and a detection limit of 0.6 µM (S/N = 3). The modified electrode exhibited advantages such as high sensitivity, a strong anti-interference capability, and good repeatability. Furthermore, the modified electrode was successfully used for DA measurement in vivo. This could present a simple reliable route for neurotransmitter detection in neuroscience.


Dopamine , Electrochemical Techniques , Electrodes , Graphite , Uric Acid , Graphite/chemistry , Uric Acid/analysis , Uric Acid/blood , Dopamine/analysis , Dopamine/blood , Electrochemical Techniques/methods , Limit of Detection , Oxidation-Reduction , Humans , Titanium/chemistry , Animals
11.
ACS Nano ; 18(20): 12808-12819, 2024 May 21.
Article En | MEDLINE | ID: mdl-38717026

Considerable progress has already been made in sweat sensors based on electrochemical methods to realize real-time monitoring of biomarkers. However, realizing long-term monitoring of multiple targets at the atomic level remains extremely challenging, in terms of designing stable solid contact (SC) interfaces and fully integrating multiple modules for large-scale applications of sweat sensors. Herein, a fully integrated wristwatch was designed using mass-manufactured sensor arrays based on hierarchical multilayer-pore cross-linked N-doped porous carbon coated by reduced graphene oxide (NPCs@rGO-950) microspheres with high hydrophobicity as core SC, and highly selective monitoring simultaneously for K+, Na+, and Ca2+ ions in human sweat was achieved, exhibiting near-Nernst responses almost without forming an interfacial water layer. Combined with computed tomography, solid-solid interface potential diffusion simulation results reveal extremely low interface diffusion potential and high interface capacitance (598 µF), ensuring the excellent potential stability, reversibility, repeatability, and selectivity of sensor arrays. The developed highly integrated-multiplexed wristwatch with multiple modules, including SC, sensor array, microfluidic chip, signal transduction, signal processing, and data visualization, achieved reliable real-time monitoring for K+, Na+, and Ca2+ ion concentrations in sweat. Ingenious material design, scalable sensor fabrication, and electrical integration of multimodule wearables lay the foundation for developing reliable sweat-sensing systems for health monitoring.


Electrolytes , Graphite , Sweat , Wearable Electronic Devices , Sweat/chemistry , Humans , Graphite/chemistry , Electrolytes/chemistry , Ions/analysis , Calcium/analysis , Sodium/analysis , Sodium/chemistry , Biosensing Techniques/instrumentation , Electrochemical Techniques/instrumentation , Electrochemical Techniques/methods , Potassium/analysis
12.
Langmuir ; 40(20): 10634-10647, 2024 May 21.
Article En | MEDLINE | ID: mdl-38723623

Hematin, an iron-containing porphyrin compound, plays a crucial role in various biological processes, including oxygen transport, storage, and functionality of the malarial parasite. Specifically, hematin-Fe interacts with the nitrogen atom of antimalarial drugs, forming an intermediate step crucial for their function. The electron transfer functionality of hematin in biological systems has been scarcely investigated. In this study, we developed a biomimicking electrical wiring of hematin-Fe with a model N-drug system, represented as {hematin-Fe---N-drug}. We achieved this by immobilizing hematin on a multiwalled carbon nanotube (MWCNT)/N-graphene quantum dot (N-GQD) modified electrode (MWCNT/N-GQD@Hemat). N-GQD serves as a model molecular drug system containing nitrogen atoms to mimic the {hematin-Fe---N-drug} interaction. The prepared bioelectrode exhibited a distinct redox peak at a measured potential (E1/2) of -0.410 V vs Ag/AgCl, accompanied by a surface excess value of 3.54 × 10-9 mol cm-2. This observation contrasts significantly with the weak or electroinactive electrochemical responses documented in literature-based hematin systems. We performed a comprehensive set of physicochemical and electrochemical characterizations on the MWCNT/N-GQD@Hemat system, employing techniques including FESEM, TEM, Raman spectroscopy, IR spectroscopy, and AFM. To evaluate the biomimetic electrode's electroactivity, we investigated the selective-mediated reduction of H2O2 as a model system. As an important aspect of our research, we demonstrated the use of scanning electrochemical microscopy to visualize the in situ electron transfer reaction of the biomimicking electrode. In an independent study, we showed enzyme-less electrocatalytic reduction and selective electrocatalytic sensing of H2O2 with a detection limit of 319 nM. We achieved this using a batch injection analysis-coupled disposable screen-printed electrode system in physiological solution.


Hemin , Hydrogen Peroxide , Nanotubes, Carbon , Oxidation-Reduction , Hydrogen Peroxide/chemistry , Hemin/chemistry , Nanotubes, Carbon/chemistry , Electrodes , Graphite/chemistry , Quantum Dots/chemistry , Nitrogen/chemistry , Surface Properties , Electrochemical Techniques/methods , Catalysis
13.
ACS Appl Mater Interfaces ; 16(20): 26943-26953, 2024 May 22.
Article En | MEDLINE | ID: mdl-38718354

The continuous, noninvasive monitoring of human blood pressure (BP) through the accurate detection of pulse waves has extremely stringent requirements on the sensitivity and stability of flexible strain sensors. In this study, a new ultrasensitive flexible strain sensor based on the interlayer synergistic effect was fabricated through drop-casting and drying silver nanowires and graphene films on polydimethylsiloxane substrates and was further successfully applied for continuous monitoring of BP. This strain sensor exhibited ultrahigh sensitivity with a maximum gauge factor of 34357.2 (∼700% sensitivity enhancement over other major sensors), satisfactory response time (∼85 ms), wide strange range (12%), and excellent stability. An interlayer fracture mechanism was proposed to elucidate the working principle of the strain sensor. The real-time BP values can be obtained by analyzing the relationship between the BP and the pulse transit time. To verify our strain sensor for real-time BP monitoring, our strain sensor was compared with a conventional electrocardiogram-photoplethysmograph method and a commercial cuff-based device and showed similar measurement results to BP values from both methods, with only minor differences of 0.693, 0.073, and 0.566 mmHg in the systolic BP, diastolic BP, and mean arterial pressure, respectively. Furthermore, the reliability of the strain sensors was validated by testing 20 human subjects for more than 50 min. This ultrasensitive strain sensor provides a new pathway for continuous and noninvasive BP monitoring.


Nanowires , Silver , Humans , Nanowires/chemistry , Silver/chemistry , Blood Pressure/physiology , Graphite/chemistry , Blood Pressure Determination/instrumentation , Blood Pressure Determination/methods , Male , Dimethylpolysiloxanes/chemistry , Nanostructures/chemistry , Adult
14.
ACS Appl Mater Interfaces ; 16(20): 25601-25609, 2024 May 22.
Article En | MEDLINE | ID: mdl-38727578

We report an ultrasensitive sandwich-type electrochemical immunosensor to detect the breast cancer biomarker CA 15-3. Amine-functionalized composite of reduced graphene oxide and Fe3O4 nanoparticles (MRGO-NH2) was used as an electrochemical sensing platform material to modify the electrodes. The nanocomposite comprising Pt and Fe3O4 nanoparticles (NPs) anchored on multiwalled carbon nanotubes (Pt-Fe3O4-MWCNTs-NH2) was utilized as a pseudoenzymatic signal-amplifying label. Compared to reduced graphene oxide, the composite MRGO-NH2 platform material demonstrated a higher electrochemical signal. In the Pt-Fe3O4-MWCNTs-NH2 label, multiwalled carbon nanotubes provided the substratum to anchor abundant catalytic Pt and Fe3O4 NPs. The nanocomposites were thoroughly characterized using transmission electron microscopy, Fourier transform infrared spectroscopy, X-ray diffraction, scanning electron microscopy, and X-ray photoelectron spectroscopy. An electroanalytical study and prevalidation of the immunosensor was carried out. The immunosensor exhibited exceptional capabilities in detecting CA 15-3, offering a wider linear range of 0.0005-100 U mL-1 and a lower detection limit of 0.00008 U mL-1. Moreover, the designed immunosensor showed good specificity, reproducibility, and acceptable stability. The sensor was successfully applied to analyze samples from breast cancer patients, yielding reliable results.


Biomarkers, Tumor , Breast Neoplasms , Electrochemical Techniques , Nanocomposites , Nanotubes, Carbon , Platinum , Humans , Nanotubes, Carbon/chemistry , Breast Neoplasms/diagnosis , Nanocomposites/chemistry , Electrochemical Techniques/methods , Biomarkers, Tumor/analysis , Biomarkers, Tumor/blood , Female , Platinum/chemistry , Biosensing Techniques/methods , Graphite/chemistry , Amines/chemistry , Mucin-1/analysis , Mucin-1/blood , Immunoassay/methods , Limit of Detection
15.
J Nanobiotechnology ; 22(1): 240, 2024 May 12.
Article En | MEDLINE | ID: mdl-38735931

Zinc oxide nanoparticles (ZnO NPs) stand as among the most significant metal oxide nanoparticles in trigger the formation of reactive oxygen species (ROS) and induce apoptosis. Nevertheless, the utilization of ZnO NPs has been limited by the shallowness of short-wavelength light and the constrained production of ROS. To overcome these limitations, a strategy involves achieving a red shift towards the near-infrared (NIR) light spectrum, promoting the separation and restraining the recombination of electron-hole (e--h+) pairs. Herein, the hybrid plasmonic system Au@ZnO (AZ) with graphene quantum dots (GQDs) doping (AZG) nano heterostructures is rationally designed for optimal NIR-driven cancer treatment. Significantly, a multifold increase in ROS generation can be achieved through the following creative initiatives: (i) plasmonic Au nanorods expands the photocatalytic capabilities of AZG into the NIR domain, offering a foundation for NIR-induced ROS generation for clinical utilization; (ii) elaborate design of mesoporous core-shell AZ structures facilitates the redistribution of electron-hole pairs; (iii) the incorporation GQDs in mesoporous structure could efficiently restrain the recombination of the e--h+ pairs; (iv) Modification of hyaluronic acid (HA) can enhance CD44 receptor mediated targeted triple-negative breast cancer (TNBC). In addition, the introduced Au NRs present as catalysts for enhancing photothermal therapy (PTT), effectively inducing apoptosis in tumor cells. The resulting HA-modified AZG (AZGH) exhibits efficient hot electron injection and e--h+ separation, affording unparalleled convenience for ROS production and enabling NIR-induced PDT for the cancer treanment. As a result, our well-designed mesoporous core-shell AZGH hybrid as photosensitizers can exhibit excellent PDT efficacy.


Gold , Graphite , Oxidative Stress , Quantum Dots , Reactive Oxygen Species , Triple Negative Breast Neoplasms , Zinc Oxide , Triple Negative Breast Neoplasms/drug therapy , Reactive Oxygen Species/metabolism , Humans , Oxidative Stress/drug effects , Female , Cell Line, Tumor , Gold/chemistry , Graphite/chemistry , Zinc Oxide/chemistry , Animals , Quantum Dots/chemistry , Mice , Metal Nanoparticles/chemistry , Apoptosis/drug effects , Hyaluronic Acid/chemistry , Electrons
16.
ACS Appl Mater Interfaces ; 16(19): 25169-25180, 2024 May 15.
Article En | MEDLINE | ID: mdl-38695741

Additive manufacturing holds promise for rapid prototyping and low-cost production of biosensors for diverse pathogens. Among additive manufacturing methods, screen printing is particularly desirable for high-throughput production of sensing platforms. However, this technique needs to be combined with carefully formulated inks, rapid postprocessing, and selective functionalization to meet all requirements for high-performance biosensing applications. Here, we present screen-printed graphene electrodes that are processed with thermal annealing to achieve high surface area and electrical conductivity for sensitive biodetection via electrochemical impedance spectroscopy. As a proof-of-concept, this biosensing platform is utilized for electrochemical detection of SARS-CoV-2. To ensure reliable specificity in the presence of multiple variants, biolayer interferometry (BLI) is used as a label-free and dynamic screening method to identify optimal antibodies for concurrent affinity to the Spike S1 proteins of Delta, Omicron, and Wild Type SARS-CoV-2 variants while maintaining low affinity to competing pathogens such as Influenza H1N1. The BLI-identified antibodies are robustly bound to the graphene electrode surface via oxygen moieties that are introduced during the thermal annealing process. The resulting electrochemical immunosensors achieve superior metrics including rapid detection (55 s readout following 15 min of incubation), low limits of detection (approaching 500 ag/mL for the Omicron variant), and high selectivity toward multiple variants. Importantly, the sensors perform well on clinical saliva samples detecting as few as 103 copies/mL of SARS-CoV-2 Omicron, following CDC protocols. The combination of the screen-printed graphene sensing platform and effective antibody selection using BLI can be generalized to a wide range of point-of-care immunosensors.


Biosensing Techniques , Graphite , Interferometry , SARS-CoV-2 , Spike Glycoprotein, Coronavirus , Graphite/chemistry , SARS-CoV-2/isolation & purification , SARS-CoV-2/immunology , Biosensing Techniques/methods , Humans , Interferometry/instrumentation , Spike Glycoprotein, Coronavirus/immunology , COVID-19/diagnosis , COVID-19/virology , Electrodes , Electrochemical Techniques/methods , Influenza A Virus, H1N1 Subtype/isolation & purification , Influenza A Virus, H1N1 Subtype/immunology
17.
J Phys Chem Lett ; 15(19): 5120-5129, 2024 May 16.
Article En | MEDLINE | ID: mdl-38709198

In the past few decades, nanometer-scale pores have been employed as powerful tools for sensing biological molecules. Owing to its unique structure and properties, solid-state nanopores provide interesting opportunities for the development of DNA sequencing technology. Controlling DNA translocation in nanopores is an important means of improving the accuracy of sequencing. Here we present a proof of principle study of accelerating DNA captured across targeted graphene nanopores using surface charge density and find the intrinsic mechanism of the combination of electroosmotic flow induced by charges of nanopore and electrostatic attraction/repulsion between the nanopore and ssDNA. The theoretical study performed here provides a new means for controlling DNA transport dynamics and makes better and cheaper application of graphene in molecular sequencing.


DNA , Graphite , Nanopores , Static Electricity , Graphite/chemistry , DNA/chemistry , DNA, Single-Stranded/chemistry , Electroosmosis , Sequence Analysis, DNA/methods
18.
J Phys Chem B ; 128(19): 4751-4758, 2024 May 16.
Article En | MEDLINE | ID: mdl-38709975

The surface patterning in natural systems has exhibited appreciable functional advantages for life activities, which serve as inspiration for the design of artificial counterparts to achieve functions such as directional liquid transport at the nanoscale. Here, we propose a patterned two-dimensional (2D) in-plane heterostructure with a triangle-shaped hexagonal boron nitride (hBN) track embedded in graphene nanosheets, which can achieve unidirectional and self-propelled transport of nanodroplets carrying various biomolecules such as DNA, RNA, and peptides. Our extensive MD simulations show that the wettability gradient on the patterned heterostructure can drive the motion of nanodroplet with an instantaneous acceleration, which also permits long-distance transport (>100 nm) at the microsecond time scale. The different behaviors of various types of biomolecules have been further studied systematically within the transporting nanodroplets. These findings suggest that these specially designed, patterned heterostructures have the potential for spontaneous, directional transport of important biomolecules, which might be useful in biosensing, drug delivery, and biomedical nanodevices.


Boron Compounds , DNA , Graphite , Molecular Dynamics Simulation , Graphite/chemistry , DNA/chemistry , Boron Compounds/chemistry , Nanostructures/chemistry , RNA/chemistry , Peptides/chemistry , Wettability
19.
Sci Rep ; 14(1): 10293, 2024 05 04.
Article En | MEDLINE | ID: mdl-38704412

In this study, a sensitive and selective fluorescent chemosensor was developed for the determination of pirimicarb pesticide by adopting the surface molecular imprinting approach. The magnetic molecularly imprinted polymer (MIP) nanocomposite was prepared using pirimicarb as the template molecule, CuFe2O4 nanoparticles, and graphene quantum dots as a fluorophore (MIP-CuFe2O4/GQDs). It was then characterized using X-ray diffraction (XRD) technique, Fourier transforms infrared (FT-IR) spectroscopy, scanning electron microscope (SEM), and transmission electron microscopy (TEM). The response surface methodology (RSM) was also employed to optimize and estimate the effective parameters of pirimicarb adsorption by this polymer. According to the experimental results, the average particle size and imprinting factor (IF) of this polymer are 53.61 nm and 2.48, respectively. Moreover, this polymer has an excellent ability to adsorb pirimicarb with a removal percentage of 99.92 at pH = 7.54, initial pirimicarb concentration = 10.17 mg/L, polymer dosage = 840 mg/L, and contact time = 6.15 min. The detection of pirimicarb was performed by fluorescence spectroscopy at a concentration range of 0-50 mg/L, and a sensitivity of 15.808 a.u/mg and a limit of detection of 1.79 mg/L were obtained. Real samples with RSD less than 2 were measured using this chemosensor. Besides, the proposed chemosensor demonstrated remarkable selectivity by checking some other insecticides with similar and different molecular structures to pirimicarb, such as diazinon, deltamethrin, and chlorpyrifos.


Pesticides , Pyrimidines , Pesticides/analysis , Carbamates/analysis , Carbamates/chemistry , Quantum Dots/chemistry , Molecularly Imprinted Polymers/chemistry , Polymers/chemistry , Spectrometry, Fluorescence/methods , Graphite/chemistry , Molecular Imprinting/methods , Adsorption , Limit of Detection , Spectroscopy, Fourier Transform Infrared , Nanocomposites/chemistry , Nanocomposites/ultrastructure
20.
Anal Chim Acta ; 1306: 342581, 2024 Jun 01.
Article En | MEDLINE | ID: mdl-38692785

Cancer detection is still a major challenge in public health. Identification of oncogene is the first step toward solving this problem. Studies have revealed that various cancers are associated with miRNA expression. Therefore, the sensitive detection of miRNA is substantially important to solve the cancer problem. In this study, let-7a, a representative substance of miRNA, was selected as the detection target. With the assistance of magnetic beads commonly used in biosensors and self-synthesized graphene oxide materials, specificity and sensitivity detection of the target gene let-7a were achieved via protease-free signal amplification. The limit of detection (LOD) was as low as 15.015pM. The fluorescence signal intensity showed a good linear relationship with the logarithm of let-7a concentration. The biosensor could also detect let-7a in complex human serum samples. Overall, this fluorescent biosensor is not only simple to operate, but also strongly specificity to detect let-7a. Therefore, it has substantial potential for application in the early diagnosis of clinical medicine and biological research.


Biosensing Techniques , Graphite , Limit of Detection , MicroRNAs , Biosensing Techniques/methods , Humans , Graphite/chemistry , MicroRNAs/analysis , MicroRNAs/blood , Spectrometry, Fluorescence , Fluorescent Dyes/chemistry , Neoplasms/diagnosis , Neoplasms/blood
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