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1.
Des Monomers Polym ; 27(1): 35-50, 2024.
Article in English | MEDLINE | ID: mdl-38903406

ABSTRACT

The C3-symmetry ionic polymer PPyTri has been designed with multi-walled carbon nanotubes (MWCNTs) or graphene nanoplatelets (GNPs) and studied as an ultrasensitive electrochemical sensor for trace Hg(II) detection. The synthesis approach incorporated attaching three pyridinium cationic components with chloride anions to the triazine core. The precursors, BPy, were synthesized using a condensation process involving 4-pyridine carboxaldehyde and focused nicotinic hydrazide. The polymer PPyTri was further modified with either MWCNTs or GNPs. The resulting ionic polymer PPyTri and its fabricated nanocomposites were characterized using infrared (IR), nuclear magnetic resonance (NMR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and powder X-ray diffraction (XRD). The analysis revealed that both the polymer and its nanocomposites have semi-crystalline structures. The electroactivity of the designed nanocomposites toward Hg + 2 ions revealed that among the nanocomposites and bare copolymer, the glassy carbon electrode (GCE) adapted with the PPyTri GNPs-5% exhibited the greatest current response over a wide range of Hg + 2 concentrations. The nanocomposite-modified electrode presented an excellent sensitivity of 83.33 µAµM - 1 cm - 2, a low detection limit of 0.033 nM, and a linear dynamic range of 0.1 nM to 0.01 mM (R2 = 0.9945).

2.
Talanta ; 278: 126456, 2024 Jun 22.
Article in English | MEDLINE | ID: mdl-38917551

ABSTRACT

Bimetallic lanthanide metal-organic frameworks (bi-Ln-MOFs) exhibit great appeal for ratiometric luminescent sensors due to their unique advantages. Specially, the low-lying energy of the empty 4f band of Ce4+ ions benefits Ce-MOFs with robust and broad fluorescent emission. Therefore, constructing ratiometric sensors based on Ce-MOFs is of significance but remains a challenge. Here, a two-dimensional (2D) bi-Ln-MOF is fabricated using Eu3+/Ce4+ and 5-boronoisophthalic acid (5-bop) via a crystal phase transformation strategy to construct a ratiometric luminescent Hg2+ sensor. Due to the lower energy gap of Ce4+ compared to Eu3+ and the corresponding stronger energy-absorption ability, the Ce4+ in bi-Ln-MOF shows a stronger and broader fluorescent emission than that of Eu3+. The substitution of the boric acid group in the bi-Ln-MOF by Hg2+ amplifies the difference between the two lanthanide ions. Therefore, the fluorescence intensity of Ce4+ increases whereas that of Eu3+ decreases accordingly, a behavior distinct from individual Eu-MOF or Ce-MOF performance. This novel bi-Ln-MOF sensor not only achieves a wide linear response range from 0.5 to 120 µM with a low detection limit of 167 nM for Hg2+, but also demonstrates exceptional selectivity and stability. The intriguing sensing mechanism of energy competition and the novel synthesis approach for 2D bi-Ln-MOF are anticipated to broaden the application possibilities of bi-Ln-MOFs for designing ratiometric sensors.

3.
Chempluschem ; : e202400203, 2024 May 10.
Article in English | MEDLINE | ID: mdl-38728531

ABSTRACT

A dyad Carbazolyl-bis(hydrazinobenzothiazole) was designed to form a symmetrical structure that containing two-arm active binding sites facilitates coordination with Hg2+ ion. This sensor has imparted a colorimetric and fluorometric changes in presence of Hg2+ ions. The ligand showed a selective blue shift in presence of Hg2+even in co-existence with heavy metal ions with luminescence change from colorless to blue and colorless to green under day light. Enhanced Intramolecular charge transfer process is responsible for fluorescence transformation when ligand interacts with Hg2+ ion. The emission spectra showed a ratiometric response to increasing addition of Hg2+ ions. The sensor is capable of detecting above the lower concentration of 6.8025×10-8 M. The fluorescence efficiency of CBT-2 with Hg2+ ion is quite stable under different co-metal ions and wide range of pH 6 to 9. The sensor CBT-2 forms a 1 : 1 stoichiometric complex with Hg2+ ions and the binding nature is confirmed from the 1H-NMR, FTIR, and mass spectroscopic studies. The sensor CBT-2 and its Hg2+ complex possess good binding nature to protein in Bovine Serum Albumin which could be good in biological applications. Additionally, wedevelop a practical application in real water sample analysis and electrochemical detection via oxidation potential discrimination.

4.
Environ Sci Pollut Res Int ; 31(26): 38196-38216, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38795297

ABSTRACT

Finding a cost-effective, efficient, and environmentally friendly technique for the removal of mercury ion (Hg2+) in water and wastewater can be a challenging task. This paper presents a novel and efficient adsorbent known as the graphene oxide-Cu2SnS3-polyaniline (GO-CTS-PANI) nanocomposite, which was synthesised and utilised to eliminate Hg2+ from water samples. The soft-soft interaction between Hg2+ and sulphur atoms besides chelating interaction between -N and Hg2+ is the main mechanism for Hg2+ adsorption onto the GO-CTS-PANI adsorbent. Various characterisation techniques, including Fourier transform infrared spectrophotometry (FT-IR), field emission scanning electron microscopy (FESEM), energy-dispersive X-ray spectroscopy (EDX), transmission electron microscopy (TEM), elemental mapping analysis, and X-ray diffraction analysis (XRD), were employed to analyse the adsorbent. The Box-Behnken method, utilising Design Expert Version 7.0.0, was employed to optimise the crucial factors influencing the adsorption process, such as pH, adsorbent quantity, and contact time. The results indicated that the most efficient adsorption occurred at pH 6.5, with 12 mg of GO-CTS-PANI adsorbent, and 30-min contact time that results in a maximum removal rate of 95% for 50 mg/L Hg2+ ions. The study also investigated the isotherm and kinetics of the adsorption process that the adsorption of Hg2+ onto the adsorbent happened in sequential layers (Freundlich isotherm) and followed by the pseudo-second-order kinetic model. Furthermore, response surface methodology (RSM) analysis indicates that pH is the most influential parameter in enhancing adsorption efficiency. In addition to traditional models, this study employed some artificial intelligence (AI) methods including the Random Forest algorithm to enhance the prediction of adsorption process efficiency. The findings demonstrated that the Random Forest algorithm exhibited high accuracy with a correlation coefficient of 0.98 between actual and predicted adsorption rates. This study highlights the potential of the GO-CTS-PANI nanocomposite for effectively removing of Hg2+ ions from water resources.


Subject(s)
Aniline Compounds , Graphite , Mercury , Nanocomposites , Water Pollutants, Chemical , Mercury/chemistry , Graphite/chemistry , Nanocomposites/chemistry , Adsorption , Aniline Compounds/chemistry , Water Pollutants, Chemical/chemistry , Kinetics , Copper/chemistry , Water Purification/methods
5.
Spectrochim Acta A Mol Biomol Spectrosc ; 318: 124530, 2024 Oct 05.
Article in English | MEDLINE | ID: mdl-38805990

ABSTRACT

Mercury ion (Hg2+) is one of the most threatening substances to human health, and the mercury poisoning can damage physiological homeostasis severely in human, even cause death. Intriguingly, Sulfur dioxide (SO2), a gas signal molecule in human, can specifically interact with Hg2+ for relieving mercury poisoning. However, the dynamic interaction of Hg2+ with SO2 at the tempospatial level and the correlation between Hg2+ and SO2 in the pathological process of mercury poisoning are still elusive. Herein, we rationally designed a reversible and dual color fluorescent probe (CCS) for dynamically visualizing Hg2+ and SO2 and deciphering their interrelationship in mercury poisoning. CCS held good sensitivity, selectivity and reversibility to Hg2+ and SO2, that enabled CCS to specifically detect SO2 and Hg2+ via cyan fluorescence channel (centered around 485 nm) and red fluorescence channel (centered around 679 nm), respectively. Notably, the separate fluorescence signal changes of CCS realized the dynamic tracing of Hg2+ and SO2 in living cells, and presented the potential for exploring the correlation between SO2 and Hg2+ in mercury poisoning.


Subject(s)
Fluorescent Dyes , Mercury , Spectrometry, Fluorescence , Sulfur Dioxide , Mercury/analysis , Humans , Sulfur Dioxide/analysis , Sulfur Dioxide/metabolism , Fluorescent Dyes/chemistry , HeLa Cells , Color , Fluorescence
6.
Anal Chim Acta ; 1309: 342685, 2024 Jun 22.
Article in English | MEDLINE | ID: mdl-38772667

ABSTRACT

The monitoring of heavy metal ions in ocean is crucial for environment protection and assessment of seawater quality. However, the detection of heavy metal ions in seawater with electrochemical sensors, especially for long-term monitoring, always faces challenges due to marine biofouling caused by the nonspecific adsorption of microbial and biomolecules. Herein, an electrochemical aptasensor, integrating both antifouling and antibacterial properties, was developed for the detection of Hg2+ in the ocean. In this electrochemical aptasensor, eco-friendly peptides with superior hydrophilicity served as anti-biofouling materials, preventing nonspecific adsorption on the sensing interface, while silver nanoparticles were employed to eliminate bacteria. Subsequently, a ferrocene-modified aptamer was employed for the specific recognition of Hg2+, leveraging the aptamer's ability to fold into a thymine-Hg2+-thymine (T-Hg2+-T) structure upon interaction, and bringing ferrocene nearer to the sensor surface, significantly amplifying the electrochemical response. The prepared electrochemical aptasensor significantly reduced the nonspecific adsorption in seawater while maintaining sensitive electrochemical response. Furthermore, the biosensor exhibited a linear response range of 0.01-100 nM with a detection limit of 2.30 pM, and realized the accurate monitoring of mercury ions in real marine environment. The research results offer new insights into the preparation of marine antifouling sensing devices, and it is expected that sensors with antifouling and antimicrobial capabilities will find broad applications in the monitoring of marine pollutants.


Subject(s)
Anti-Bacterial Agents , Biofouling , Biosensing Techniques , Electrochemical Techniques , Mercury , Seawater , Mercury/analysis , Seawater/chemistry , Seawater/microbiology , Electrochemical Techniques/methods , Anti-Bacterial Agents/analysis , Anti-Bacterial Agents/pharmacology , Biosensing Techniques/methods , Biofouling/prevention & control , Aptamers, Nucleotide/chemistry , Silver/chemistry , Water Pollutants, Chemical/analysis , Metal Nanoparticles/chemistry , Limit of Detection , Ferrous Compounds/chemistry , Metallocenes
7.
Spectrochim Acta A Mol Biomol Spectrosc ; 318: 124484, 2024 Oct 05.
Article in English | MEDLINE | ID: mdl-38788504

ABSTRACT

A novel rhodamine-based multi-ion fluorescent sensor, RGN, was designed and synthesized for the highly selective detection of mercury ions (Hg2+) in ethanol and water systems, as well as trivalent cations (Fe3+, Al3+, and Cr3+) in acetonitrile and water systems using a two-step Schiff base reaction method. Nuclear magnetic titration experiments and theoretical calculations demonstrated that the sensor achieved the detection of the aforementioned metal ions through the fluorescence turn-on phenomenon induced by lactam ring-opening. Density functional theory (DFT) calculation results showed decreased HOMO-LUMO energy gaps and increased dipole moments, indicating the effective coordination of the sensor with the corresponding metal ions to form more stable complexes, thereby achieving detection objectives. Furthermore, the fluorescence turn-on sensor RGN exhibited relatively low detection limits, with limits of detection (LOD) for Fe3+, Al3+, Cr3+, and Hg2+ being 10.20 nM, 14.66 nM, 58.78 nM, and 73.33 nM, respectively. Finally, practical applications of sensor RGN in environmental water samples, L929 cells, and zebrafish were demonstrated, indicating its potential for detecting and tracking Fe3+, Al3+, Cr3+, and Hg2+ in environmental samples and biological systems, with prospects for biomedical applications in the diagnosis and treatment of heavy metal ion-induced diseases.


Subject(s)
Fluorescent Dyes , Mercury , Rhodamines , Spectrometry, Fluorescence , Zebrafish , Rhodamines/chemistry , Mercury/analysis , Animals , Fluorescent Dyes/chemistry , Fluorescent Dyes/chemical synthesis , Spectrometry, Fluorescence/methods , Mice , Limit of Detection , Chromium/analysis , Aluminum/analysis , Iron/analysis , Iron/chemistry , Density Functional Theory , Cell Line , Optical Imaging
8.
Food Chem ; 450: 139261, 2024 Aug 30.
Article in English | MEDLINE | ID: mdl-38657344

ABSTRACT

This study employed an innovative copper oxide/cuprous oxide (CuO/Cu2O) polyhedron­cadmium sulphide quantum dots (CdS QDs) double Z-scheme heterostructure as a matrix for the cathodic PEC determination of mercury ions (Hg2+). First, the CuO/Cu2O polyhedral composite was prepared by calcining a copper-based metal organic framework (Cu-MOF). Subsequently, the amino-modified CuO/Cu2O was integrated with mercaptopropionic acid (MPA)-capped CdS QDs to form a CuO/Cu2O polyhedron-CdS QDs double Z-scheme heterostructure, producing a strong cathodic photocurrent. Importantly, this heterostructure exhibited a specifically reduced photocurrent for Hg2+ when using CdS QDs as Hg2+-recognition probe. This was attributed to the extreme destruction of the double Z-scheme heterostructure and the in situ formation of the CuO/Cu2O-CdS/HgS heterostructure. Besides, p-type HgS competed with the matrix for electron acceptors, further decreasing the photocurrent. Consequently, Hg2+ was sensitively assayed, with a low detection limit (0.11 pM). The as-prepared PEC sensor was also used to analyse Hg2+ in food and the environment.


Subject(s)
Cadmium Compounds , Copper , Electrochemical Techniques , Mercury , Metal-Organic Frameworks , Quantum Dots , Sulfides , Quantum Dots/chemistry , Copper/chemistry , Mercury/analysis , Mercury/chemistry , Sulfides/chemistry , Cadmium Compounds/chemistry , Electrochemical Techniques/instrumentation , Metal-Organic Frameworks/chemistry , Food Contamination/analysis , Electrodes , Limit of Detection
9.
J Hazard Mater ; 470: 134269, 2024 May 15.
Article in English | MEDLINE | ID: mdl-38613952

ABSTRACT

Mercury (Hg) is one of the most widespread pollutants that pose serious threats to public health and the environment. People are inevitably exposed to Hg via different routes, such as respiration, dermal contact, drinking or diet. Hg poisoning could cause gingivitis, inflammation, vomiting and diarrhea, respiratory distress or even death. Especially during the developmental stage, there is considerable harm to the brain development of young children, causing serious symptoms such as intellectual disability and motor impairments, and delayed neural development. Therefore, it's of great significance to develop a specific, quick, practical and labor-saving assay for monitoring Hg2+. Herein, a mitochondria-targeted dual (excitation 700 nm and emission 728 nm) near-infrared (NIR) fluorescent probe JZ-1 was synthesized to detect Hg2+, which is a turn-on fluorescent probe designed based on the rhodamine fluorophore thiolactone, with advantages of swift response, great selectivity, and robust anti-interference capability. Cell fluorescence imaging results showed that JZ-1 could selectively target mitochondria in HeLa cells and monitor exogenous Hg2+. More importantly, JZ-1 has been successfully used to monitor gastrointestinal damage of acute mercury poisoning in a drug-induced mouse model, which provided a great method for sensing Hg species in living subjects, as well as for prenatal diagnosis.


Subject(s)
Fluorescent Dyes , Mercury Poisoning , Mercury , Mitochondria , Fluorescent Dyes/chemistry , Mitochondria/drug effects , Humans , Animals , HeLa Cells , Mercury Poisoning/diagnostic imaging , Mercury/toxicity , Optical Imaging , Mice , Gastrointestinal Tract/drug effects , Gastrointestinal Tract/diagnostic imaging , Gastrointestinal Tract/metabolism , Female , Gastrointestinal Diseases/diagnostic imaging , Gastrointestinal Diseases/chemically induced , Rhodamines/chemistry , Rhodamines/toxicity
10.
J Fluoresc ; 2024 Mar 08.
Article in English | MEDLINE | ID: mdl-38457076

ABSTRACT

Herein, a fluorescent "on-off-on" nanosensor based on N,S-CDs was developed for highly precise and sensitive recognition of Hg2+ and ampicillin (AMP). Nitrogen and sulfur co-doped carbon dots with blue fluorescence were synthesized by one-pot hydrothermal method using ammonium citrate and DL-methionine as precursors. N,S-CDs exhibited a surface abundant in -OH, -COOH, and -NH2 groups, aiding in creating non-fluorescent ground state complexes when combined with Hg2+, leading to the suppression of N,S-CDs' fluorescence. Subsequent to additional AMP application, the mixed system's fluorescence was restored. Based on this N,S-CDs sensing system, the thresholds for detection for AMP and Hg2+ were discovered to be 0.121 µM and 0.493 µM, respectively. Furthermore, this methodology proved effective in identifying AMP in real samples of tap and lake water, yielding satisfactory results. Consequently, in the area of bioanalysis in intricate environmental sample work, the sensing system showed tremendous promise.

11.
Talanta ; 273: 125843, 2024 Jun 01.
Article in English | MEDLINE | ID: mdl-38492285

ABSTRACT

Ligand-protected gold nanoclusters (AuNCs) have become promising nanomaterials in fluorescence (FL) methods for mercury ions (Hg2+) monitoring, but low FL efficiency hinders their widespread application. Herein, AuNCs/cerium-based metal-organic frameworks (AuNCs/Ce-MOFs) were prepared by loading 6-aza-2-thiothymine-protected AuNCs (ATT-AuNCs) with aggregation-induced emission (AIE) effect on the surface of Ce-MOFs by electrostatic attraction. This strategy improved the FL intensity of AuNCs through two aspects: (i) the AIE effect of ATT-AuNCs and (ii) the confinement effect of Ce-MOFs, which improved the restriction of intramolecular motion (RIM) of ATT-AuNCs. In addition, Ce-MOFs could adsorb and aggregate Hg2+ during detection, which might increase the local concentration. Therefore, based on the high FL signal of AuNCs/Ce-MOFs and enriched Hg2+, sensitive detection of Hg2+ could be achieved. More importantly, the strong specific recognition between AuNCs and Hg2+ could guarantee selectivity. The developed FL sensor exhibited superior detection performances with a wide linear range of 0.2-500 ng mL-1 and a low detection limit of 0.067 ng mL-1. Furthermore, the FL sensor used for sensitive and selective detection of Hg2+ in real samples, and the results agreed well with the standard method. In summary, this work proposed an effective and generalized strategy for improving the FL efficiency of AuNCs, which would greatly facilitate their application in pollutant monitoring.

12.
Int J Mol Sci ; 25(6)2024 Mar 10.
Article in English | MEDLINE | ID: mdl-38542159

ABSTRACT

This article discusses the design and analysis of a new chemical chemosensor for detecting mercury(II) ions. The chemosensor is a hydrazone made from 4-methylthiazole-5-carbaldehyde and fluorescein hydrazide. The structure of the chemosensor was confirmed using various methods, including nuclear magnetic resonance spectroscopy, infrared spectroscopy with Fourier transformation, mass spectroscopy, and quantum chemical calculations. The sensor's ability in the highly selective and sensitive discovery of Hg2+ ions in water was demonstrated. The detection limit for mercury(II) ions was determined to be 0.23 µM. The new chemosensor was also used to detect Hg2+ ions in real samples and living cells using fluorescence spectroscopy. Chemosensor 1 and its complex with Hg2+ demonstrate a significant tendency to enter and accumulate in cells even at very low concentrations.


Subject(s)
Mercury , Metals, Heavy , Water Pollutants, Chemical , Fluorescein , Water , Fluorescent Dyes/chemistry , Water Pollutants, Chemical/analysis , Mercury/analysis , Spectrometry, Fluorescence/methods
13.
J Fluoresc ; 2024 Mar 02.
Article in English | MEDLINE | ID: mdl-38430416

ABSTRACT

Here, straightforward and environmentally friendly fluorescent nitrogen doped carbon quantum dots (N-CQDs) with a high blue fluorescence emission at 455 nm are used for ultrasensitive Hg2+ ion detection. Folic acid and urea are used as carbon sources in the carbonization process. Two broad absorption bands at around 280 and 370 nm from UV-Vis spectrum and characteristic absorption peaks from infrared spectrum confirms the successful synthesis of the N-CQDs. Energy dispersive X-Ray analysis confirmed the elemental composition of the N-CQDs. Transmission electron microscopy showed the homogeneous globular morphology of the N-CQDs with an average particle size of 65 nm. Zeta potential measurement established the stability and surface charge of N-CQDs. Dynamic light scattering measurement showed the average size of N-CQDs. With the addition of Hg2+ ion to N-CQDs, the blue fluorescence emission is quenched. Moreover, the N-CQDs can be applied to real water sample such as pond water, river water, and tap water. The detection limit is approximately calculated to be 12 nM and linear range is 0-30 parts per billion.

14.
J Fluoresc ; 2024 Feb 02.
Article in English | MEDLINE | ID: mdl-38305987

ABSTRACT

In this paper, we obtained nitrogen and phosphorus co-doped carbon dots through a hydrothermal method using o-phenylenediamine and citric acid in a 40% phosphoric acid environment. The carbon dots emitted fluorescence at 476 nm under excitation at 408 nm and exhibited good selectivity and high sensitivity towards mercury ions. These carbon dots showed excellent dispersibility in water and maintained stable fluorescence even in high concentration salt environments. The interaction between mercury ions and functional groups on the carbon dots surface through electrostatic interaction resulted in static quenching. Simultaneously, by detecting the lifetime and transient absorption spectra of the carbon dots, we observed that the coordination of mercury ions with the carbon dots broadened the band structure of the carbon dots, and the existing photoinduced electron transfer process increased the non-radiative transition channel. The combined effect of dynamic quenching and static quenching significantly reduced the fluorescence intensity of the carbon dots at 476 nm. The carbon dots exhibited linear detection of mercury ions in the range of 0.01-1 µM, with a detection limit as low as 0.0245 µM. In terms of practical water environmental detection applications, these carbon dots were able to effectively detect mercury ions in tap water and lake water, demonstrating their broad application prospects in the field of environmental metal analysis.

15.
Anal Chim Acta ; 1287: 342132, 2024 Jan 25.
Article in English | MEDLINE | ID: mdl-38182354

ABSTRACT

BACKGROUND: Recently, headspace single-drop microextraction (HS-SDME) has attracted some attention for developing sensitive and selective colorimetric assays due to its excellent capability to reduce matrix interference and enrich analytes. However, the single droplet limits direct visual observation of color change and its quantitative measurement suffers from reduced optical path length. Therefore, amplifying the detection signals in both volume and intensity is an important and challenging task for improving the sensitivity, stability, and accuracy of such colorimetric analysis. RESULTS: In this study, a "headspace-nanoenzyme" (HS-NE) strategy was proposed that successfully addressed these challenges and enabled the colorimetric and fluorescent dual-mode detection of trace Hg2+. Atomic Hg0, generated via chemical vapor generation (CVG), underwent headspace reaction with AuNPs droplet to form Au@HgNPs, thus catalyzing the oxidation of o-phenylenediamine (OPD) in the presence of H2O2. The absorbance and fluorescence intensity of oxidized OPD were proportion to the concentration of Hg2+ in the sample solution. Due to the greatly enhanced peroxidase-like activity by Au@HgNPs, the limit of detection was as low as 0.98 nM and 0.21 nM for the colorimetric and fluorescent modes, respectively. The applicability of this assay was further demonstrated with determination of Hg2+ in real environmental and biological samples. Moreover, a convenient and cost-effective paper-based sensing platform was fabricated for rapid on-site detection of Hg2+. SIGNIFICANCE AND NOVELTY: This novel HS-NE strategy combines HS-SDME and nanoenzyme-based sensing to achieve dual effects of eliminating matrix interference and amplifying the measurement signal, resulting in improved accuracy, enhanced stability, high sensitivity, and exceptional selectivity, with great potential for on-site determination of trace Hg2+.


Subject(s)
Mercury , Metal Nanoparticles , Colorimetry , Gold , Hydrogen Peroxide , Coloring Agents , Peroxidases
16.
Biosens Bioelectron ; 249: 116039, 2024 Apr 01.
Article in English | MEDLINE | ID: mdl-38241797

ABSTRACT

DNA nanostructures are emerging as promising biosensing platforms due to their programmability, predictable assembly, and compatibility with aptamers for enhanced selectivity. This study focuses on a triple-multivalent aptamer (tApt) complex immobilized on a tetrahedral DNA nanostructure (TDN) and integrated with an electrochemically reduced graphene oxide (ERGO) electrode for highly sensitive mercury ion (Hg2+) detection. Compared to a linear multivalent aptamer-modified electrode (S2/ERGO-GCE), the 3D tApt/ERGO-GCE aptasensor exhibits superior sensitivity, signal amplification, and reaction kinetics. The tApt/ERGO-GCE sensor achieves an exceptional limit of detection (LOD) of 4.1 zM, surpassing the LOD of 0.71 fM for S2/ERGO-GCE. Additionally, the tApt/ERGO-GCE sensor demonstrates faster response times, with a half-saturation time (T1/2) of 6 minutes compared to 17 minutes for S2/ERGO/GCE. The 3D tApt aptamer's superior performance is attributed to its tetrahedral DNA structure integrated on ERGO, providing multiple aptamer binding sites, facilitating oriented immobilization on the electrode surface, and enhancing analyte capture and concentration. In contrast, the linear S2 aptamers lack rigidity, resulting in a disordered orientation on the electrode surface, hindering efficient Hg2+ binding and reducing target molecule binding efficiency. This study underscores the potential of triple-multivalent aptamer-based nanostructures for ultrasensitive and rapid biosensing applications. The tApt/ERGO-GCE aptasensor's exceptional sensitivity, signal amplification, and reaction kinetics make it a promising tool for Hg2+ detection and other biosensing applications.


Subject(s)
Aptamers, Nucleotide , Biosensing Techniques , Graphite , Mercury , Nanocomposites , Electrochemical Techniques/methods , Biosensing Techniques/methods , Oligonucleotides , Graphite/chemistry , DNA , Electrodes , Nanocomposites/chemistry , Aptamers, Nucleotide/chemistry
17.
J Fluoresc ; 34(2): 905-913, 2024 Mar.
Article in English | MEDLINE | ID: mdl-37418199

ABSTRACT

With the expansion of human activities, the consequent influx of mercury (Hg) into the food chain and the environment is seriously threatening human life. Herein, nitrogen and sulfur co-doped fluorescent carbon quantum dots (yCQDs) were prepared via a hydrothermal method using o-phenylenediamine (OPD) and taurine as precursors. The morphological characteristics as well as spectral features of yCQDs indicated that the photoluminescence mechanism should be the molecular state fluorophores of 2, 3-diaminophenothiazine (oxOPD), which is the oxide of OPD. The as-synthesized yCQDs exhibited sensitive recognition of Hg2+. According to the investigation in combination of UV-Vis absorption spectra, time-resolved fluorescence spectra and quantum chemical calculations, the abundant functional groups on the surface of yCQDs allowed Hg2+ to bind with yCQDs through various interactions, and the formed complexes significantly inhibited the absorption of excitation light, resulting in the static fluorescence quenching of yCQDs. The proposed yCQDs was utilized for Hg2+ sensing with the limit of detection calculated to be 4.50 × 10- 8 M. Furthermore, the recognition ability of yCQDs for Hg2+ was estimated in tap water, lake water and bottled water, and the results indicated that yCQDs have potential applications in monitoring Hg2+.

18.
Luminescence ; 39(1): e4615, 2024 Jan.
Article in English | MEDLINE | ID: mdl-37957886

ABSTRACT

By using the method of low-temperature crystallization, CsPbBr3 perovskite nanocrystals (PNCs) coated with trifluoroacetyl lysine (Tfa-Lys) and oleamine (Olam) were synthesized in aqueous solution. The structure of the CsPbBr3 PNCs was characterized by many methods, such as ultraviolet (UV)-visible absorption spectrophotometer, fluorescence spectrophotometer, transmission electron microscopy (TEM), and X-ray diffraction (XRD) pattern. The fluorescence emission of the CsPbBr3 PNCs is stable in water for about 1 day at room temperature. It was also found that the fluorescence of the PNCs could be obviously and selectively quenched after the addition of mercury ion (Hg2+ ), allowing a visual detection of Hg2+ by the naked eye under UV light illumination. The fluorescence quenching rate (I0 /I) has a good linear relationship with the addition of Hg2+ in the concentration range 0.075 to 1.5 mg/L, with a correlation coefficient (R2 ) of 0.997, and limit of detection of 0.046 mg/L. The fluorescence quenching mechanism of the PNCs was determined by the fluorescence lifetime and X-ray photoelectron spectroscopy (XPS) of the PNCs. Overall, the synthesis method for CsPbBr3 PNCs is simple and rapid, and the as-prepared PNCs are stable in water that could be conveniently used for selective detection of Hg2+ in the water environment.


Subject(s)
Calcium Compounds , Mercury , Nanoparticles , Titanium , Water/chemistry , Oxides/chemistry , Nanoparticles/chemistry
19.
Environ Sci Pollut Res Int ; 31(3): 4318-4329, 2024 Jan.
Article in English | MEDLINE | ID: mdl-38100024

ABSTRACT

Mercury ion (Hg2+) is a highly toxic and ubiquitous pollutant, whose effective detection has aroused widespread concern. A novel ratiometric fluorescent sensor has been designed to rapidly and efficiently detect Hg2+ based on blue/red carbon dots (CDs) with environmental friendliness. This sensor was well characterized via TEM, FTIR, XPS, UV-vis, and zeta potential analysis and displayed excellent fluorescence properties and stability. The fluorescence of blue CDs at 447 nm was significantly quenched with the addition of Hg2+ resulted from the static quenching, whereas that of red CDs at 650 nm remained invariable. A sensitive method for Hg2+ determination was constructed in the range of 0.05-7.0 nmol mL-1 with optimal conditions, and the detection limit was down to 0.028 nmol mL-1. Meanwhile, compared to other 17 metal ions, the ratiometric fluorescent sensor exhibited high selectivity for Hg2+. Furthermore, satisfied recoveries had also been obtained for measuring trace Hg2+ in practical environmental samples. This developed ratiometric fluorescent sensor provided a reliable, environmental-friendly, rapid, and efficient platform for the detection of Hg2+ in environmental applications.


Subject(s)
Mercury , Quantum Dots , Spectrometry, Fluorescence/methods , Mercury/analysis , Fluorescent Dyes , Carbon , Ions , Limit of Detection
20.
Food Chem ; 440: 138185, 2024 May 15.
Article in English | MEDLINE | ID: mdl-38100966

ABSTRACT

A sensitive electrochemical assay for simultaneously detecting cadmium ion (Cd2+) and mercury ion (Hg2+) with the aptamer as recognition unit was established, in which methylene blue (MB) and target-triggered in-situ generated Ag nanoclusters (Ag NCs) were identified as signal reporters. Multi-walled carbon nanotubes and gold nanoparticles composites were prepared with polyethyleneimine to amplify electrical signals of screen-printed electrodes. Due to the particular base sequences, MB labeled Cd2+ aptamer paired with ssDNA through T-Hg-T structure with Hg2+. Notably, the C-rich structure in ssDNA acted as a template for the generation of Ag NCs, which could induce differential pulse voltammetry signals corresponding to Hg2+ concentrations. This electrochemical aptasensor exhibited detection limits of 94.01 pg/mL and 15.74 pg/mL for Cd2+ and Hg2+, respectively. The developed aptasensor allowed for practical application to tea and vegetable samples with satisfactory accuracy. This work possesses potential in developing biosensing technologies for simultaneous determination of multiple heavy metals.


Subject(s)
Aptamers, Nucleotide , Biosensing Techniques , Mercury , Metal Nanoparticles , Nanotubes, Carbon , Gold/chemistry , Cadmium , Nanotubes, Carbon/chemistry , Methylene Blue/chemistry , DNA, Single-Stranded , Electrodes , Electrochemical Techniques , Aptamers, Nucleotide/chemistry , Limit of Detection
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