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1.
J Am Chem Soc ; 2024 Jul 09.
Article in English | MEDLINE | ID: mdl-38980064

ABSTRACT

Addressing the global challenge of bacterial resistance demands innovative approaches, among which multitargeting is a widely used strategy. Current strategies of multitargeting, typically achieved through drug combinations or single agents inherently aiming at multiple targets, face challenges such as stringent pharmacokinetic and pharmacodynamic requirements and cytotoxicity concerns. In this report, we propose a bacterial-specific global disruption approach as a vastly expanded multitargeting strategy that effectively disrupts bacterial subcellular organization. This effect is achieved through a pioneering chemical design of ligand-receptor interaction-induced aggregation of small molecules, i.e., DNA-induced aggregation of a diarginine peptidomimetic within bacterial cells. These intracellular aggregates display affinity toward various proteins and thus substantially interfere with essential bacterial functions and rupture bacterial cell membranes in an "inside-out" manner, leading to robust antibacterial activities and suppression of drug resistance. Additionally, biochemical analysis of macromolecule binding affinity, cytoplasmic localization patterns, and bacterial stress responses suggests that this bacterial-specific intracellular aggregation mechanism is fundamentally different from nonselective classic DNA or membrane binding mechanisms. These mechanistic distinctions, along with the peptidomimetic's selective permeation of bacterial membranes, contribute to its favorable biocompatibility and pharmacokinetic properties, enabling its in vivo antimicrobial efficacy in several animal models, including mice-based superficial wound models, subcutaneous abscess models, and septicemia infection models. These results highlight the great promise of ligand-receptor interaction-induced intracellular aggregation in achieving a globally disruptive multitargeting effect, thereby offering potential applications in the treatment of malignant cells, including pathogens, tumor cells, and infected tissues.

2.
Sci Total Environ ; 901: 166012, 2023 Nov 25.
Article in English | MEDLINE | ID: mdl-37541517

ABSTRACT

This study provides an in-depth examination of the role of poly(lactic acid) microplastics (PLA-MPs) during sludge treatment, particularly in relation to organic compound leaching and heavy metal distribution. Through the application of advanced analytical techniques such as Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), thermal analysis, and gas chromatography-mass spectrometry (GC-MS), the release of degradation byproducts was quantified, and the effects on organic compound leaching and heavy metal distribution were assessed. Specifically, the results demonstrated that PLA-MPs significantly impacted the hydrolysis reaction, with the pH value descending in pure water as the hydrothermal temperature escalated. At 140 °C, the hydrolysate contained 20.66 % propylene ester and 16.57 % lactic acid. Furthermore, an increase in total organic carbon (TOC) was observed with increasing temperature, with TOC content at 140 °C in water almost doubling from that at 120 °C and 130 °C. With respect to heavy metals, the presence of PLA-MPs influenced the migration of Cr(VI) between solid and liquid phases in sludge. Notably, after 180 °C hydrothermal treatment, the content of Cr(VI) in the liquid phase of sludge with PLA-MPs was 9.72 %, which is higher than that of sludge without PLA-MPs at 5.80 %. These findings underline the need to consider PLA-MPs' influence on organic compound leaching and heavy metal distribution during sludge treatment.

3.
ACS Appl Mater Interfaces ; 15(16): 20458-20473, 2023 Apr 26.
Article in English | MEDLINE | ID: mdl-37039625

ABSTRACT

Bacterial biofilms are major causes of persistent and recurrent infections and implant failures. Biofilms are formable by most clinically important pathogens worldwide, such as Staphylococcus aureus, Pseudomonas aeruginosa, and Escherichia coli, causing recalcitrance to standard antibiotic therapy or anti-biofilm strategies due to amphiphilic impermeable extracellular polymeric substances (EPS) and the presence of resistant and persistent bacteria within the biofilm matrix. Herein, we report our design of an oligoamidine-based amphiphilic "nano-sword" with high structural compacity and rigidity. Its rigid, amphiphilic structure ensures effective penetration into EPS, and the membrane-DNA dual-targeting mechanism exerts strong bactericidal effect on the dormant bacterial persisters within biofilms. The potency of this oligoamidine is shown in two distinct modes of application: it may be used as a coating agent for polycaprolactone to fully inhibit surface biofilm growth in an implant-site mimicking micro-environment; meanwhile, it cures model mice of biofilm infections in various ex vivo and in vivo studies.


Subject(s)
Biofilms , Staphylococcal Infections , Mice , Animals , Extracellular Polymeric Substance Matrix , Staphylococcus aureus , Staphylococcal Infections/drug therapy , Anti-Bacterial Agents/pharmacology , Bacteria , Escherichia coli , Pseudomonas aeruginosa
4.
Environ Res ; 216(Pt 2): 114532, 2023 01 01.
Article in English | MEDLINE | ID: mdl-36243048

ABSTRACT

Microplastics' (MPs) aging process and environmental behavior have attracted extensive attention due to the potential long-term ecological impact. MPs enriched in sludge may accelerate aging during sludge treatment and the affecting environmental behavior, i.e., adsorption performance for pollutants. However, the related studies have not been well researched, especially for the biodegradable MPs. This study revealed the influences of hydrothermal treatment on the characteristics of polylactic acid microplastics (PLA-MPs) and the consequences on heavy metals adsorption. The changes in PLA-MPs' physiochemical properties were characterized and compared. PLA-MPs' surface became irregular, and the oxygen-containing functional groups increased through FTIR and XPS analysis. Meanwhile, the molecular weight and crystallinity of PLA-MPs decreased significantly with the rising in hydrothermal temperature. Accordingly, the adsorption capacity of PLA-MPs for Pb2+ increased from 93.97 µg g-1 for the raw PLA-MPs to 1058.03 µg g-1 for the aged PLA-MPs. Multiple adsorption kinetics and isotherms were discussed for the Pb2+ adsorption onto PLA-MPs with different aging of the PLA-MPs. The adsorption mechanisms of Pb2+ relate to electrostatic interaction and complexation. The main difference is that the adsorption for raw PLA-MPs is dominated by physical and chemical adsorption, whereas the adsorption for the aged PLA-MPs prefers chemical adsorption. In addition, we carefully evaluated the influences of pH, dissolved organic matter, and ionic strength on the PLA-MPs adsorption. The present study highlighted the significance of hydrothermal treatment on the MPs aging and the adsorption performance.


Subject(s)
Metals, Heavy , Water Pollutants, Chemical , Microplastics , Sewage , Plastics , Adsorption , Lead , Metals, Heavy/chemistry , Polyesters , Water Pollutants, Chemical/analysis
5.
Front Pediatr ; 10: 1036565, 2022.
Article in English | MEDLINE | ID: mdl-36440338

ABSTRACT

Objective: To evaluate the effects of antenatal corticosteroids (ACS) on blood glucose fluctuations in late-preterm neonates. Methods: A retrospective study was performed on 236 neonates with gestational age of 34+0 to 36+6 weeks who were admitted to the neonatology department of a tertiary general hospital in China's Zhejiang Province between April 2020 and February 2022. The neonates were divided into three groups: complete course, partial course, and control. Primary outcome was the neonatal blood glucose levels within the first 48 h of life. Results: 134 (56.8%) newborns were exposed to a complete course of ACS, 56 (23.7%) had a to a partial course of ACS, and 46 (19.5%) had no exposure to ACS. The patients in the complete course group had the highest proportion of neonatal hypoglycemia (16.4% vs. 3.6% and 6.5%).The patients exposed to a complete course of dexamethasone had significantly lower blood glucose levels within 12 h of birth than the control group, although no significant differences were observed after 24 h. Differences in blood glucose levels were more significant among male infants, although blood glucose curves of the male and female infants remained close to the overall trend. Conclusions: Blood glucose levels in late-preterm neonates may decrease after ACS administration, especially after exposure to a complete course. The effects are more pronounced in the first 12 h of life, with males being more severely affected; however, the effects on blood glucose levels were not significant 24 h after birth. This can provide a reference for future clinical studies.

6.
ACS Chem Biol ; 17(11): 3178-3190, 2022 11 18.
Article in English | MEDLINE | ID: mdl-36269311

ABSTRACT

Most Gram-positive-selective antibiotics have low activity against Gram-negative bacteria due to the presence of an outer membrane barrier. There is, therefore, interest in developing combination therapies that can penetrate the outer membrane (OM) with known antibiotics coupled with membrane-active sensitizing adjuvants. However, two unanswered questions hinder the development of such combination therapies: the sensitization spectrum of the sensitizer and the mechanism of antibiotic-sensitizer mutual potentiation. Here, with pentamidine as an example, we screened a library of 170 FDA-approved antibiotics in combination with pentamidine, a compound known to disturb the OM of Gram-negative bacteria. We found that four antibiotics, minocycline, linezolid, valnemulin, and nadifloxacin, displaced enhanced activity in combination with pentamidine against several multidrug-resistant Gram-negative bacteria. Through a descriptor-based structural-activity analysis and multiple cell-based biochemical assays, we found that hydrophobicity, partial charge, rigidity, and surface rugosity were key factors that affected sensitization via a cooperative membrane damage mechanism in which lipopolysaccharides and phospholipids were identified as sites of synergy. Finally, in vitro experiments showed that the linezolid-pentamidine combination slowed the generation of drug resistance, and there was also potent activity in in vivo experiments. Overall, our results highlight the importance of the physicochemical properties of antibiotics and cooperative membrane damage for synergistic pentamidine-antibiotic drug combinations.


Subject(s)
Anti-Bacterial Agents , Pentamidine , Anti-Bacterial Agents/pharmacology , Anti-Bacterial Agents/chemistry , Pentamidine/pharmacology , Linezolid/pharmacology , Gram-Negative Bacteria , Drug Resistance, Multiple, Bacterial , Microbial Sensitivity Tests
7.
J Am Chem Soc ; 144(23): 10622-10639, 2022 06 15.
Article in English | MEDLINE | ID: mdl-35657057

ABSTRACT

Gram-negative bacteria, especially the ones with multidrug resistance, post dire challenges to antibiotic treatments due to the presence of the outer membrane (OM), which blocks the entry of many antibiotics. Current solutions for such permeability issues, namely lipophilic-cationic derivatization of antibiotics and sensitization with membrane-active agents, cannot effectively potentiate the large, globular, and hydrophilic antibiotics such as vancomycin, due to ineffective disruption of the OM. Here, we present our solution for high-degree OM binding of vancomycin via a hybrid "derivatization-for-sensitization" approach, which features a combination of LPS-targeting lipo-cationic modifications on vancomycin and OM disruption activity from a sensitizing adjuvant. 106- to 107-fold potentiation of vancomycin and 20-fold increase of the sensitizer's effectiveness were achieved with a combination of a vancomycin derivative and its sensitizer. Such potentiation is the result of direct membrane lysis through cooperative membrane binding for the sensitizer-antibiotic complex, which strongly promotes the uptake of vancomycin and adds to the extensive antiresistance effectiveness. The potential of such derivatization-for-sensitization approach was also supported by the combination's potent in vivo antimicrobial efficacy in mouse model studies, and the expanded application of such strategy on other antibiotics and sensitizer structures.


Subject(s)
Gram-Negative Bacteria , Vancomycin , Animals , Anti-Bacterial Agents/pharmacology , Mice , Microbial Sensitivity Tests , Vancomycin/pharmacology
8.
Adv Healthc Mater ; 11(15): e2200546, 2022 08.
Article in English | MEDLINE | ID: mdl-35545965

ABSTRACT

Antimicrobial peptidomimetics (AMPMs) have received widespread attention as potentially powerful weapons against antibiotic resistance. However, AMPMs' membrane disruption mechanism not only brings resistance-resistant nature, but also nonspecific binding and disruption toward eukaryotic cell membranes, and consequently, their hemolytic activity is the primary concern on clinical applications. Here, the preparation and screening of an AMPM library is reported, through which a best-performing hit, PT-b1, can be obtained. To further improve PT-b1's hemocompatibility, a strategy is devised to mask the amphiphilicity of the AMPM using a charge-free, FDA-approved amphiphilic polymer, Pluronic F-127 (PF127). A PF127 solution containing PT-b1 can form a temperature-sensitive, absorbable hydrogel at higher concentration, but dissolve and complex with PT-b1 through hydrophobic interactions at lower concentration or lower temperature. The complexation from PF127 can mask the amphiphilicity of PT-b1 and render it extremely hemocompatible, yet the reversibility in such nanocomplexation and the existence of a secondary mechanism of action ensure that the AMPM's potency remains unchanged. The in vivo effectiveness of this antimicrobial hydrogel system is demonstrated using a mice wound infection model established with Methicillin-resistant Staphylococcus aureus, and observations indicate the hydrogel can promote wound healing and suppress bacteria-caused inflammation even when resistant pathogens are involved.


Subject(s)
Anti-Infective Agents , Methicillin-Resistant Staphylococcus aureus , Peptidomimetics , Animals , Anti-Bacterial Agents/chemistry , Anti-Infective Agents/chemistry , Hydrogels/pharmacology , Mice , Microbial Sensitivity Tests , Poloxamer , Polymers/pharmacology
9.
Chemosphere ; 286(Pt 3): 131810, 2022 Jan.
Article in English | MEDLINE | ID: mdl-34399259

ABSTRACT

In this study, the composite materials using different ratios of biochar (BC) to nano-hydroxyapatite (nHAP) were prepared for the remediation of lead (Pb) and cadmium (Cd) contaminated water and soil. The sorption and the immobilization experiments indicated a higher sorption capacity and immobilization efficiency of Pb compared to those of Cd. The characteristics of XRD, FTIR, SEM, and XPS manifested that dissolution-precipitation, cation exchange, complexation, and cation-π interaction were the main four mechanisms for the sorption of Pb2+ and Cd2+ using composite material PC1 (nHAP/BC = 1/1). From semi-quantitative analysis, the mineral effect accounted for the majority of the immobilization of Pb and Cd. Due to obvious Pb-precipitates in the sorbed material, dissolution-precipitation primarily affected the sorption of Pb using PC1, while the immobilization of Cd was mainly attributable to cation exchange. Such results corresponded to the stable Pb-precipitates and unstable Cd-compounds in soil, among which the latter was prone to be released into the environment. The sorption capacity in aqueous solutions and the immobilization efficiencies in the soil for both Pb and Cd increased with the addition of nHAP, which were linearly correlated to the nHAP proportion in the composite materials. In future practical applications, the percentages of composite materials can be designed according to the specific pollutant concentration. This study sheds light on the explicit immobilization mechanisms for Pb and Cd in aqueous solutions to better understand their behaviors in the soil remediated by relevant materials.


Subject(s)
Cadmium , Soil Pollutants , Adsorption , Charcoal , Durapatite , Lead , Soil , Soil Pollutants/analysis , Water
10.
Biomaterials ; 275: 120858, 2021 08.
Article in English | MEDLINE | ID: mdl-34044257

ABSTRACT

The increasing number of infections caused by multi-drug resistance (MDR) bacteria is an omen of a new global challenge. As one of the countermeasures under development, antimicrobial peptides (AMPs) and AMP mimics have emerged as a new family of antimicrobial agents with high potential, due to their low resistance generation rate and effectiveness against MDR bacterial strains resulted from their membrane-disrupting mechanism of action. However, most reported AMPs and AMP mimics have facially amphiphilic structures, which may lead to undesired self-aggregation and non-specific binding, as well as increased cytotoxicity toward mammalian cells, all of which put significant limits on their applications. Here, we report an oligomer with the size of short AMPs, with both hydrophobic carbon chain and cationic groups placed on its backbone, giving an alternatingly amphiphilic structure that brings better selectivity between mammalian and bacterial cell membranes. In addition, the oligomer shows affinity toward DNA, thus it can utilize bacterial DNA located in the vulnerable nucleoid as the second drug target. Benefiting from these designs, the oligomer shows higher therapeutic index and synergistic effect with other antibiotics, while its low resistance generation rate and effectiveness on multi-drug resistant bacterial strains can be maintained. We demonstrate that this alternatingly amphiphilic, DNA-binding oligomer is not only resistance-resistant, but is also able to selectively eliminate bacteria at the presence of mammalian cells. Importantly, the oligomer exhibits good in vivo activity: it cleans all bacteria on Caenorhabditis elegans without causing apparent toxicity, and significantly improves the survival rate of mice with severely infected wounds in a mice excision wound model study.


Subject(s)
Anti-Infective Agents , Antimicrobial Cationic Peptides , Animals , Anti-Bacterial Agents/pharmacology , Anti-Infective Agents/pharmacology , Drug Resistance, Multiple, Bacterial , Mice , Microbial Sensitivity Tests
11.
Sci Adv ; 7(5)2021 01.
Article in English | MEDLINE | ID: mdl-33571116

ABSTRACT

Antibiotic resistance is now a major threat to human health, and one approach to combating this threat is to develop resistance-resistant antibiotics. Synthetic antimicrobial polymers are generally resistance resistant, having good activity with low resistance rates but usually with low therapeutic indices. Here, we report our solution to this problem by introducing dual-selective mechanisms of action to a short amidine-rich polymer, which can simultaneously disrupt bacterial membranes and bind to bacterial DNA. The oligoamidine shows unobservable resistance generation but high therapeutic indices against many bacterial types, such as ESKAPE strains and clinical isolates resistant to multiple drugs, including colistin. The oligomer exhibited excellent effectiveness in various model systems, killing extracellular or intracellular bacteria in the presence of mammalian cells, removing all bacteria from Caenorhabditis elegans, and rescuing mice with severe infections. This "dual mechanisms of action" approach may be a general strategy for future development of antimicrobial polymers.

12.
Chemosphere ; 253: 126661, 2020 Aug.
Article in English | MEDLINE | ID: mdl-32278913

ABSTRACT

Nano-hydroxyapatite (nHAP) has an excellent effect on the remediation of Pb contaminated water and soil. In this study, an efficient modified nHAP was prepared assisted with two-stage ultrasonic irradiation. The effects of ultrasound modification on the nHAP were tested using X-ray diffraction (XRD), Scanning Electron Microscopy (SEM), Fourier Transform InfraRed spectroscopy (FTIR), Brunauer-Emmett-Teller (BET) and combined batch Pb uptake experiments. The nHAP with ultrasound has a fine structure with the width and length of around 9 nm and 40 nm respectively. The ultrasound parameter of 1s/36s in stage 1 and 16s/18s in stage 2 was verified as the optimum under which the nHAP prepared performed the best with the maximum adsorption capacity of 1300.93 mg/g. The results of XRD and SEM indicated that the sorbent after uptake of Pb2+ was mainly Pb10(PO4)6OH2 (HPY) with insignificant Ca10Pb10-x(PO4)6OH2. Compared the results of Pb/Ca, pH and XRD with the metal fraction of Pb in adsorbents during the dynamic sorption process, this research proved that the effects of complexation, cation exchange and dissolution and precipitation coexisted in the initial stage, while the dissolution and precipitation gradually dominated the adsorption mechanism with contact time. The processes of Pb2+ uptake by nHAP sorbents prepared under different ultrasound parameter presented almost the same dynamic mechanism with a little difference in time node. The research of dynamic mechanism of Pb2+ uptake by a superior nHAP is essential for both contaminated water and soil remediation.


Subject(s)
Durapatite/chemistry , Environmental Pollutants/chemistry , Environmental Restoration and Remediation/methods , Lead/chemistry , Adsorption , Soil/chemistry , Soil Pollutants/analysis , Spectroscopy, Fourier Transform Infrared , Ultrasonic Waves , X-Ray Diffraction
13.
Luminescence ; 27(6): 466-72, 2012.
Article in English | MEDLINE | ID: mdl-22223590

ABSTRACT

A highly sensitive flow-injection chemiluminescence (FIA-CL) method based on the CdTe nanocrystals and potassium permanganate chemiluminescence system was developed for the determination of L-ascorbic acid. It was found that sodium hexametaphosphate (SP), as an enhancer, could increase the chemiluminescence (CL) emission from the redox reaction of CdTe quantum dots with potassium permanganate in near-neutral pH conditions. L-ascorbic acid is suggested as a sensitive enhancer for use in the above energy-transfer excitation process. Under optimal conditions, the calibration graph of emission intensity against logarithmic l-ascorbic acid concentration was linear in the range 1.0 × 10(-9)-5.0 × 10(-6) mol/L, with a correlation coefficient of 0.9969 and relative standard deviation (RSD) of 2.3% (n = 7) at 5.0 × 10(-7) mol/L. The method was successfully used to determine L-ascorbic acid in vitamin C tablets. The possible mechanism of the chemiluminescence in the system is also discussed.


Subject(s)
Ascorbic Acid/analysis , Cadmium Compounds/chemistry , Luminescence , Luminescent Measurements/methods , Phosphates/chemistry , Potassium Permanganate/chemistry , Tellurium/chemistry , Calibration , Glutathione/chemistry , Hydrogen-Ion Concentration , Microscopy, Electron, Transmission , Nanoparticles/chemistry , Quantum Dots , Tablets/analysis , Thioacetamide/chemistry , Vegetables/chemistry
14.
Anal Chim Acta ; 713: 111-4, 2012 Feb 03.
Article in English | MEDLINE | ID: mdl-22200316

ABSTRACT

Based on NaYF(4):Yb(3+), Er(3+) upconversion nanocrystals as donor and 4-((4-(2-aminoethylamino)naphthalen-1-yl)diazenyl) benzenesulfonic acid dihydrochloride (ANDBS) as acceptor, an efficient luminescence energy transfer (LET) system was developed for selective and sensitive determination of trace amounts of nitrite. Based on Griess Reaction, ANDBS was generated by the quantitative reaction of nitrite, sulfanilamide and N-(1-naphtyl)-ethylenediamine dihydrochloride (N1NED). The degree of the overlaps between the emission spectrum of NaYF(4):Yb(3+), Er(3+) and the absorption spectrum of ANDBS were effective for luminescence energy transfer. Under the optimal condition, the upconversion luminescence quenching of NaYF(4):Yb(3+), Er(3+) was in proportion to the trace amounts of nitrite. The detection limit for nitrite achieved is 0.0046 µg mL(-1) and the system shows high sensitivity towards nitrite at 0.008000-0.2500 µg mL(-1) range.

15.
Luminescence ; 26(6): 434-8, 2011.
Article in English | MEDLINE | ID: mdl-20872915

ABSTRACT

Based on the fluorescence quenching of Terbium (III)-sodium hexametaphosphate (Tb/SHMP) chelates in the presence chromate (III), a sensitive fluorimetric method was developed for the determination of trace amounts of chromium (III) in aqueous solutions. Under the optimum conditions, the linear calibration graph was obtained (R = 0.996). The linear range and detection limit of Cr (III) were 7.69 × 10(-7) to 1.15 × 10(-4) mol L(-1) and 4.50 × 10(-7) mol L(-1), respectively. The proposed method had a wider linear range and was proved to be very sensitive, rapid and simple. The method was applied successfully to the determination of chromium (III) in the synthetic samples and real water samples. Moreover, the reaction mechanism was discussed through the fluorescence lifetime and proved to be dynamic quenching behavior.


Subject(s)
Chelating Agents/chemistry , Chromates/analysis , Fluorescent Dyes/chemistry , Organometallic Compounds/chemistry , Buffers , Calibration , Hydrogen-Ion Concentration , Limit of Detection
16.
Article in English | MEDLINE | ID: mdl-21081282

ABSTRACT

The sensitized fluorescence intensity of the terbium (III) ion can be notably enhanced in the presence of sodium hexametaphosphate (SHMP). Based on this, water-soluble Tb-SHMP chelate complexes were synthesized in aqueous solutions, and characterized by spectrofluorometry. 6-Mercapto-5-triazole[4,3-b]-S-tetrazine was generated by the quantitative reaction of HCHO with 4-amino-3-hydrazino-5-mercapto-1,2,4-triazole under alkaline conditions at room temperature. The spectral overlap between the emission of Tb-SHMP chelate complexes and absorption of 6-mercapto-5-triazole[4,3-b]-S-tetrazine meets the prerequisite for fluorescence energy transfer. Based on this, a novel efficient fluorescence energy transfer system between Tb-SHMP chelate complexes as donor and 6-mercapto-5-triazole[4,3-b]-S-tetrazine as acceptor was developed for the determination of HCHO in aqueous solutions. Under the optimal experimental conditions, this method is capable of detecting HCHO concentrations from 2.06×10(-5) to 6.18×10(-3) mg mL(-1) and the limit of detection was 7.11×10(-6) mg mL(-1). Compared with other general methods for the determination of HCHO, the proposed method improved the sensitivity and selectivity. Moreover, the proposed method was successfully applied to the determination of HCHO in water samples.


Subject(s)
Chelating Agents/chemistry , Energy Transfer , Formaldehyde/analysis , Terbium/chemistry , Water/chemistry , Ions , Phosphates/chemistry , Solutions , Spectrometry, Fluorescence , Sulfhydryl Compounds/chemistry , Temperature , Time Factors
17.
Talanta ; 83(1): 139-44, 2010 Nov 15.
Article in English | MEDLINE | ID: mdl-21035654

ABSTRACT

With the biomolecule glutathione (GSH) as a capping ligand, Eu(3+)-doped cadmium sulfide composite nanoparticles were successfully synthesized through a straightforward one-pot process. An efficient fluorescence energy transfer system with CdS nanoparticles as energy donor and Eu(3+) ions as energy accepter was developed. As a result of specific interaction, the fluorescence intensity of Eu(3+)-doped CdS nanoparticles is obviously reduced in the presence of Hg(2+). Moreover, the long fluorescent lifetime and large Stoke's shift of europium complex permit sensitive fluorescence detection. Under the optimal conditions, the fluorescence intensity of Eu(3+) at 614 nm decreased linearly with the concentration of Hg(2+) ranging from 10 nmol L(-1) to 1500 nmol L(-1), the limit of detection for Hg(2+) was 0.25 nmol L(-1). In addition to high stability and reproducibility, the composite nanoparticles show a unique selectivity towards Hg(2+) ion with respect to common coexisting cations. Moreover, the developed method was applied to the detection of trace Hg(2+) in aqueous solutions. The probable mechanism of reaction between Eu(3+)-doped CdS composite nanoparticles and Hg(2+) was also discussed.


Subject(s)
Cadmium Compounds/chemistry , Cations, Divalent/analysis , Europium/chemistry , Fluorescence Resonance Energy Transfer/methods , Mercury/analysis , Nanoparticles/chemistry , Sulfides/chemistry , Glutathione/chemistry , Sensitivity and Specificity
18.
Spectrochim Acta A Mol Biomol Spectrosc ; 77(3): 625-9, 2010 Oct 15.
Article in English | MEDLINE | ID: mdl-20663708

ABSTRACT

A fluorescent probe for mercury(II) ions, based on the quenching of fluorescence of terbium(III) ions doped in CdS nanoparticles, has been developed. The terbium(III)-doped cadmium sulfide composite nanoparticles were successfully synthesized through a straightforward one-pot process, with the biomolecule glutathione (GSH) as a capping ligand. In addition, the terbium(III) ions were observed an enhancement of emission intensity, owing to fluorescence energy transfer from the excited CdS particles to the emitting terbium(III). Because of a specific interaction, the fluorescence intensity of terbium(III)-doped CdS particles is obviously reduced in the presence of mercury(II) ions. The fluorescence quenching phenomenon of terbium(III) can be attributed to the fact that the energy transfer system was destroyed by combining with mercury(II). Under the optimal conditions, the fluorescent intensity of terbium(III) ions at 491nm decreased linearly with the concentration of mercury(II) ions ranging from 4.5nmolL(-1) to 550nmolL(-1). The limit of detection for mercury(II) was 0.1nmolL(-1). This method is simple, practical, relatively free of interference from coexisting substances and can be successfully applied to the determination of mercury(II) ions in real water samples. In addition, the probable mechanism of reaction between terbium(III)-doped CdS composite nanoparticles and mercury(II) was also discussed.


Subject(s)
Fluorescence Resonance Energy Transfer , Fluorescent Dyes/analysis , Mercury/analysis , Quantum Dots , Water Pollutants, Chemical/analysis , Cadmium Compounds , Glutathione , Hydrogen-Ion Concentration , Ligands , Limit of Detection , Microscopy, Electron, Transmission , Osmolar Concentration , Sensitivity and Specificity , Solubility , Spectrometry, Fluorescence , Spectrophotometry, Ultraviolet , Sulfides , Terbium , Water
19.
Analyst ; 135(8): 2139-43, 2010 Aug.
Article in English | MEDLINE | ID: mdl-20577665

ABSTRACT

An efficient fluorescence energy transfer (FET) system between CePO(4):Tb(3+) nanocrystals as donor and 6-mercapto-5-triazole[4,3-b]-S-tetrazine as acceptor was built. CePO(4):Tb(3+) nanocrystals were synthesized in aqueous solutions, and characterized by transmission electron microscopy, electron diffraction pattern spectroscopy and spectrofluorometry. Under alkaline conditions, 6-mercapto-5-triazole[4,3-b]-S-tetrazine was generated by redox reaction of formaldehyde (HCHO) with 4-amino-3-hydrazino-5-mercapto-1,2,4-triazole (AHMT) at room temperature. The degree of the overlap was effective for FET between the emission spectrum of CePO(4):Tb(3+) and the absorption spectrum of 6-mercapto-5-triazole[4,3-b]-S-tetrazine. Based on this system, a simple and sensitive fluorescence method for the selective determination of formaldehyde in aqueous solutions was developed. Under optimal conditions, the quenched fluorescence intensity increased linearly with the concentration of HCHO ranging from 1.03 x 10(-9) to 1.03 x 10(-5) mg mL(-1) with a correlation coefficient of 0.9976. The limit of detection was 1.65 x 10(-10) mg mL(-1). Compared with several methods, the proposed method had a wider linear range, higher selectivity and sensitivity. Moreover, analytical application of the method was demonstrated by water samples.


Subject(s)
Fluorescence Resonance Energy Transfer/methods , Formaldehyde/analysis , Solutions , Water/chemistry
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