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1.
Heliyon ; 10(14): e34657, 2024 Jul 30.
Artigo em Inglês | MEDLINE | ID: mdl-39148992

RESUMO

The capacity of South African Heulandite (HEU) zeolite to remove Pb2+ and Cd2+ ions from aqueous solution was investigated using batch experiments and molecular simulations studies. The effect of different factors on the adsorption of these ions onto the zeolite was investigated; contact time, initial metal ion concentration and the amount of HEU adsorbent. Molecular simulations was done using Monte Carlo and density functional theory. Experimental results obtained indicate that the maximum adsorption for the two ions occur at pH 5 and after 240 min of contact time. The percent removal based on contact time of Pb2+ and Cd2+ ions from water by the heulandite zeolite were 99.7 and 76.7 %, respectively. The adsorption of two metal ions onto the HEU zeolite follows the Langmuir adsorption isotherm. From the molecular simulation findings, the adsorption of Pb2+ ions onto the HEU window is equidistant from the two adjacent oxygen atoms within the HEU structure while the Cd2+ ion is adsorbed in the upper left side of the 8-ring HEU window. It was observed that the performance of the zeolite can significantly be improved by doping with germanium, aluminum, thallium indium, and sodium cations. These results indicate that the application of HEU zeolite as an adsorbent holds a great promise in heavy metal removal from aqueous solutions.

2.
Chemosphere ; : 143070, 2024 Aug 12.
Artigo em Inglês | MEDLINE | ID: mdl-39142393

RESUMO

Lead (Pb) contamination in water requires improved decontamination technologies. The addition of phosphate to precipitate Pb2⁺ is a widely used method for remediating Pb in soil and water, though it has certain limitations. This study focuses on novel 3D mesoporous layered double hydroxide (LDH) sorbents functionalized with phosphate anions for Pb2+ removal from contaminated waters. Our innovative strategy involves converting a sacrificial template MOF structure (MIL-88A(Fe)) into NixFe LDH, followed by an anion exchange reaction with phosphate anions. This process preserves the 3D microrod architecture of MIL-88A and prevents deleterious LDH particle aggregation. The synthesis results in stable microrod crystals, 1 to 2 µm long, composed of 3D assemblies of NixFe-PO4 LDH nanoplatelets with a specific surface area exceeding 110 m2/g. The novel LDH materials display fast adsorption kinetics (pseudo-second order model) and remarkably high Pb2⁺ removal performances (Langmuir isotherm model) with a capacity of 538 mg Pb2⁺/g Ni3Fe/MIL-PO4, surpassing other reported adsorbents. LDH-PO4 exhibits high selectivity for Pb2+ over competing ions like Ni2⁺ and Cd2⁺ (selectivity order is: Pb2+ > Ni2+ > Cd2+). Removal of Pb2+ from NixFeLDH/88A-PO4 involves various mechanisms, including surface complexation and surface precipitation of lead phosphate or lead hydroxide phases as revealed by structural characterization techniques.

3.
Sci Total Environ ; 950: 175190, 2024 Jul 31.
Artigo em Inglês | MEDLINE | ID: mdl-39094638

RESUMO

Lead ions are especially harmful to human health, causing significant developmental and behavioral abnormalities even at small concentrations. In real-life samples, lead ions are present in mixtures with other metal ions, creating a challenge to detect it selectively at low quantities. To address these challenges, we prepared an electrochemical sensor based on delaminated Ti3C2Tx MXene, which can selectively detect low concentrations of Pb2+ in a solution containing other common metal ions. Cyclic voltammetry was applied as an electrochemical detection method. The proposed reaction mechanism involves a reversible transition between Pb2+ ions and PbO at the MXene-based layer. The sensitivity of the sensor towards Pb2+ ions and a limit of detection were determined. The sensor, as prepared, had a linear response range within 0.15-1.0 µM, with a sensitivity of 26.7 µA/µM and LOD value of 48.7 nM, which meets the requirements set by the World Health Organization.

4.
Emerg Microbes Infect ; 13(1): 2387439, 2024 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-39139051

RESUMO

Avian influenza viruses (AIVs) are the origin of multiple mammal influenza viruses. The genetic determinants of AIVs adapted to humans have been widely elucidated, however, the molecular mechanism of cross-species transmission and adaptation of AIVs to canines are still poorly understood. In this study, two H3N2 influenza viruses isolated from a live poultry market (A/environment/Guangxi/13431/2018, GX13431) and a swab sample from a canine (A/canine/Guangdong/0601/2019, GD0601) were used to investigate the possible molecular basis that determined H3N2 AIV adapting to canine. We found that GD0601 exhibited more robust polymerase activity in cells and higher pathogenicity in mice compared with its evolution ancestor H3N2 AIV GX13431. A series of reassortments of the ribonucleoprotein (RNP) complex showed that the PB2 subunit was the crucial factor that conferred high polymerase activity of GD0601, and the substitution of I714S in the PB2 subunit of GD0601 attenuated the replication and pathogenicity in mammal cells and the mouse model. Mechanistically, the reverse mutation of I714S in the PB2 polymerase subunit which was identified in AIV GX13431 reduced the nuclear import efficiency of PB2 protein and interfered with the interactions of PB2-PA/NP that affected the assembly of the viral RNP complex. Our study reveals amino acid mutation at the position of 714 in the nuclear localization signal (NLS) area in PB2 plays an important role in overcoming the barrier from poultry to mammals of the H3N2 canine influenza virus and provides clues for further study of mammalian adaptation mechanism of AIVs.


Assuntos
Vírus da Influenza A Subtipo H3N2 , Infecções por Orthomyxoviridae , RNA Polimerase Dependente de RNA , Ribonucleoproteínas , Proteínas Virais , Animais , Cães , Vírus da Influenza A Subtipo H3N2/genética , Vírus da Influenza A Subtipo H3N2/fisiologia , Camundongos , Proteínas Virais/genética , Proteínas Virais/metabolismo , RNA Polimerase Dependente de RNA/genética , RNA Polimerase Dependente de RNA/metabolismo , Infecções por Orthomyxoviridae/virologia , Humanos , Ribonucleoproteínas/genética , Ribonucleoproteínas/metabolismo , Transporte Ativo do Núcleo Celular , Replicação Viral , Mutação , Células Madin Darby de Rim Canino , Doenças do Cão/virologia , Camundongos Endogâmicos BALB C , Células HEK293 , Vírus Reordenados/genética
5.
Int J Biol Macromol ; 277(Pt 2): 134350, 2024 Jul 31.
Artigo em Inglês | MEDLINE | ID: mdl-39094877

RESUMO

In this study, a novel and cost-effective approach was employed to prepare an effective Pb(II) adsorbent. We synthesized highly porous CMCSB-SCB microbeads with multiple active binding sites by combining carboxymethylated chitosan Schiff base (CMCSB) and sugarcane bagasse (SCB). These microbeads were structurally and morphologically characterized using various physical, analytical, and microscopic techniques. The SEM image and N2-adsorption analysis of CMCSB-SCB revealed a highly porous structure with irregularly shaped voids and interconnected pores. The CMCSB-SCB microbeads demonstrated an impressive aqueous Pb(II) adsorption capacity, reaching a maximum of 318.21 mg/g, under identified optimal conditions: pH 4.5, 15 mg microbeads dosage, 30 min contact time, and Pb(II) initial concentration (350 mg/L). The successful adsorption of Pb(II) onto CMCSB-SCB beads was validated using FTIR, EDX, and XPS techniques. Furthermore, the experimental data fitting indicated a good agreement with the Langmuir model (R2 = 0.99633), whereas the adsorption kinetics aligned well with the pseudo-second-order model (R2 = 0.99978). The study also identified the Pb(II) adsorption mechanism by CMCSB-SCB microbeads as monolayer chemisorption.

6.
Anal Chim Acta ; 1316: 342800, 2024 Aug 08.
Artigo em Inglês | MEDLINE | ID: mdl-38969435

RESUMO

Heavy metal pollution in the environment has become a significant global concern due to its detrimental effects on human health and the environment. In this study, we report an electrochemical aptasensor for the simultaneous detection of Hg2+ and Pb2+. Gold nanoflower/polyethyleneimine-reduced graphene oxide (AuNFs/PEI-rGO) was introduced on the surface of a gold electrode to improve sensing performance. The aptasensor is based on the formation of a T-Hg2+-T mismatch structure and specific cleavage of the Pb2+-dependent DNAzyme, resulting in a dual signal generated by the Exo III specific digestion of methylene blue (MB) labeled at the 3' end of probe DNA-1 and the reduction of the substrate ascorbic acid (AA) catalyzed by the signal label. The decrease of MB signal and the increase of AA oxidation peak was used to indicate the content of Hg2+ and Pb2+, respectively, with detection limits of 0.11 pM (Hg2+) and 0.093 pM (Pb2+). The aptasensor was also used for detecting Hg2+ and Pb2+ in water samples with good recoveries. Overall, this electrochemical aptasensor shows promising potential for sensitive and selective detection of heavy metals in environmental samples.


Assuntos
Aptâmeros de Nucleotídeos , Técnicas Biossensoriais , Técnicas Eletroquímicas , Exodesoxirribonucleases , Chumbo , Mercúrio , Estruturas Metalorgânicas , Poluentes Químicos da Água , Mercúrio/análise , Chumbo/análise , Chumbo/química , Estruturas Metalorgânicas/química , Aptâmeros de Nucleotídeos/química , Exodesoxirribonucleases/química , Exodesoxirribonucleases/metabolismo , Poluentes Químicos da Água/análise , Técnicas Biossensoriais/métodos , Grafite/química , Ouro/química , Limite de Detecção , Eletrodos , DNA Catalítico/química
7.
Ecotoxicol Environ Saf ; 281: 116648, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38964065

RESUMO

The pollution of Pb2+ and Cd2+ in both irrigation water and soil, coupled with the scarcity of vital mineral nutrition, poses a significant hazard to the security and quality of agricultural products. An economical potassium feldspar-derived adsorbent (PFDA) was synthesized using potassium feldspar as the main raw material through ball milling-thermal activation technology to solve this problem. The synthesis process is cost-effective and the resulting adsorbent demonstrates high efficiency in removing Pb2+ and Cd2+ from water. The removal process is endothermic, spontaneous, and stochastic, and follows the quasi-second-order kinetics, intraparticle diffusion, and Langmuir model. The adsorption and elimination of Pb2+ and Cd2+ is largely dependent on monolayer chemical sorption. The maximum removal capacity of PFDA for Pb2+ and Cd2+ at room temperature is 417 and 56.3 mg·g-1, respectively, which is superior to most mineral-based adsorbents. The desorption of Pb2+/Cd2+ on PFDA is highly challenging at pH≥3, whereas PFDA and Pb2+/Cd2+ are recyclable at pH≤0.5. When Pb2+ and Cd2+ coexisted, Pb2+ was preferentially removed by PFDA. In the case of single adsorption, Pb2+ was mainly adsorbed onto PFDA as Pb2SiO4, PbSiO3·xH2O, Pb3SiO5, PbAl2O4, PbAl2SiO6, PbAl2Si2O8, Pb2SO5, and PbSO4, whereas Cd2+ was primarily adsorbed as CdSiO3, Cd2SiO4, and Cd3Al2Si3O12. After the complex adsorption, the main products were PbSiO3·xH2O, PbAl2Si2O8, Pb2SiO4, Pb4Al2Si2O11, Pb5SiO7, PbSO4, CdSiO3, and Cd3Al2Si3O12. The forms of mineral nutrients in single and complex adsorption were different. The main mechanisms by which PFDA removed Pb2+ and Cd2+ were chemical precipitation, complexation, electrostatic attraction, and ion exchange. In irrigation water, the elimination efficiencies of Pb2+ and Cd2+ by PFDA within 10 min were 96.0 % and 70.3 %, respectively, and the concentrations of K+, Si4+, Ca2+, and Mg2+ increased by 14.0 %, 12.4 %, 55.7 %, and 878 %, respectively, within 60 min. PFDA holds great potential to replace costly methods for treating heavy metal pollution and nutrient deficiency in irrigation water, offering a sustainable, cost-effective solution and paving a new way for the comprehensive utilization of potassium feldspar.


Assuntos
Irrigação Agrícola , Cádmio , Chumbo , Poluentes Químicos da Água , Qualidade da Água , Adsorção , Poluentes Químicos da Água/química , Chumbo/química , Cádmio/química , Irrigação Agrícola/métodos , Purificação da Água/métodos , Metais Pesados/química , Compostos de Potássio/química , Nutrientes , Cinética
8.
Talanta ; 278: 126546, 2024 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-39002263

RESUMO

As a new type of porous crystalline composite material, MOF-COF has shown great advantages in metal separation. Herein, a CoMOF-COF was designed for highly selective separation of trace Pb2+ ions. The designed CoMOF-COF has a high density of nitrogen-oxygen functional groups and can selectively separate metal ions. There is a strong affinity between the designed CoMOF-COF material and metal Pb2+ ions, which can be attributed to the ordered heterogeneous porous structure and large amounts of nitrogen-and oxygen-containing functional groups. The composite showed high adsorption selectivity for Pb2+ ions and had adsorption capacity of 33 mg g-1, with high chemical stability. Based on this solid phase extraction material, a high sensitivity detection method for Pb2+ ions was established, which has the detection limit of 37.3 ng L-1, precision of 1.9 %. Linear detection range is 0.2-10 ng mL-1, and the detection of Pb2+ ions in actual water samples was realized. Through this study, it is proved that the strong affinity between the designed CoMOF-COF materials and metal Pb2+ ions can be attributed to the soft and hard acid-base theory, which reveals the structure-activity relationship between the porous heterostructure of such materials and metal separation, providing a highly selective separation material for the separation of other environmental pollutants.

9.
J Hazard Mater ; 476: 135115, 2024 Sep 05.
Artigo em Inglês | MEDLINE | ID: mdl-38976962

RESUMO

A label-free fluorescent sensing strategy for the rapid and highly sensitive detection of Pb2+ was developed by integrating Pb2+ DNAzyme-specific cleavage activity and a tetrahedral DNA nanostructure (TDN)-enhanced hyperbranched hybridization chain reaction (hHCR). This strategy provides accelerated reaction rates because of the highly effective collision probability and enriched local concentrations from the spatial confinement of the TDN, thus showing a higher detection sensitivity and a more rapid detection process. Moreover, a hairpin probe based on a G-triplex instead of a G-quadruplex or chemical modification makes hybridization chain reaction more controlled and flexible, greatly improving signal amplification capacities and eliminating labeled DNA probes. The enhanced reaction rates and improved signal amplification efficiency endowed the biosensors with high sensitivity and a rapid response. The label-free detection of Pb2+ based on G-triplex combined with thioflavin T can be achieved with a detection limit as low as 1.8 pM in 25 min. The proposed Pb2+-sensing platform was also demonstrated to be applicable for Pb2+ detection in tap water, river water, shrimp, rice, and soil samples, thus showing great potential for food safety and environmental monitoring.


Assuntos
Técnicas Biossensoriais , DNA Catalítico , Chumbo , Limite de Detecção , Hibridização de Ácido Nucleico , Chumbo/análise , Chumbo/química , DNA Catalítico/química , Técnicas Biossensoriais/métodos , Nanoestruturas/química , Poluentes Químicos da Água/análise , DNA/química , DNA/análise , Animais , Monitoramento Ambiental/métodos , Oryza/química , Poluentes Ambientais/análise
10.
Chemphyschem ; : e202400149, 2024 Jul 17.
Artigo em Inglês | MEDLINE | ID: mdl-39015100

RESUMO

The heavy metal selenophosphate Pb2P2Se6emerges as a promising room-temperature X-ray/γ-ray detectors due to its high resistivity, robust radiation-blocking capability, and outstanding carrier mobility-lifetime product, etc. However, the high activity of phosphides poses significant impediment to the synthesis and single crystal growth. In this work, we have prepared high-quality Pb2P2Se6 single crystals with using the chemical vapor transport (CVT) method. The XRD analysis combined with EDS result confirmed the uniform composition of the resulting as-grown single crystals, while UV-Vis-NIR transmittance spectra revealed the bandgap of 1.89 eV. Selected area electron diffraction patterns indicated the crystal belonged to the P21/c(14) space group. Additionally, the Au/Pb2P2Se6/Au device is fabricated, which exhibits a robust X-ray response with a sensitivity of 648.61 µC·Gy-1·cm-2 at 400 V·mm-1 under 50 kVp. Notably, the device also excels in alpha particle detection, boasting a resolution of ~14.48% under a bias of 400 V bias. The hole mobility-lifetime product (µτ)h of Pb2P2Se6 is estimated to be ~2.58×10-5 cm2·V-1. The results underscore potential applications of Pb2P2Se6 crystal is in the field of the semiconductor radiation detectors.

11.
Polymers (Basel) ; 16(11)2024 May 28.
Artigo em Inglês | MEDLINE | ID: mdl-38891469

RESUMO

This paper reports the successful development and application of an efficient method for quantifying Pb2+ in aqueous samples using a smartphone-based colorimetric device with an imprinted polymer (IIP). The IIP was synthesized by modifying the previous study; using rhodizonate, 2-acrylamido-2-methylpropane sulfonic acid (AMPS), N,N'-methylenebisacrylamide (MBA), and potassium persulfate (KPS). The polymers were then characterized. An absorption study was performed to determine the optimal conditions for the smartphone-based colorimetric device processing. The device consists of a black box (10 × 10 × 10 cm), which was designed to ensure repeatability of the image acquisition. The methodology involved the use of a smartphone camera to capture images of IIP previously exposed at Pb2+ solutions with various concentrations, and color channel values were calculated (RGB, YMK HSVI). PLS multivariate regression was performed, and the optimum working range (0-10 mg L-1) was determined using seven principal components with a detection limit (LOD) of 0.215 mg L-1 and R2 = 0.998. The applicability of a colorimetric sensor in real samples showed a coefficient of variation (% RSD) of less than 9%, and inductively coupled plasma mass spectrometry (ICP-MS) was applied as the reference method. These results confirmed that the quantitation smartphone-based colorimetric sensor is a suitable analytical tool for reliable on-site Pb2+ monitoring.

12.
Int J Biol Macromol ; 272(Pt 2): 132703, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38823744

RESUMO

Lead ion is very harmful to the environment, so it is very important to study its detection methods. In this study, a novel electrochemical sensor was constructed by modifying deoxyribonucleic acid (DNA) on the electrode, which can be used for the detection of Pb2+ in the environment. Part of the mixed solution of chitosan (CS) and Pb2+ template ions was dropped onto the surface of a glassy carbon electrode. CS-Pb2+ film was cross-linked through sodium tripolyphosphate. And a novel DNA-imprinted sensor was prepared by electrodepositing CS-Pb2+ thin film with gold nanoparticles (AuNPs), removing Pb2+ templates, and immobilizing specific double-stranded DNA. The electroactive area, surface morphology, sensitivity, and electrochemical reaction mechanism of the DNA-imprinted sensor were analyzed. The elementary reaction steps were studied through electrochemical reaction kinetics analysis. The experimental results indicate that the DNA-imprinted electrochemical biosensor can quantitatively detect Pb2+ in the range of 10-100 µM (R2 = 0.9935), and its detection limit is 6.5074 µM (3σ/slope). The sensitivity of the electrochemical biosensor is 1.55233 × 10-6 A/µM, and its active areas is 6.233 cm2. The desorption mechanism and adsorption mechanism have been explored through dynamic parameter analysis. The novel DNA imprinted electrochemical biosensor developed in this paper provides a robust method for detecting lead ions in solution. Additionally, it establishes a solid groundwork for detecting other metal ions.


Assuntos
Técnicas Biossensoriais , Quitosana , DNA , Técnicas Eletroquímicas , Ouro , Chumbo , Nanopartículas Metálicas , Impressão Molecular , Quitosana/química , Chumbo/análise , Técnicas Biossensoriais/métodos , DNA/química , DNA/análise , Ouro/química , Nanopartículas Metálicas/química , Impressão Molecular/métodos , Técnicas Eletroquímicas/métodos , Limite de Detecção , Eletrodos , Adsorção
13.
Sci Total Environ ; 945: 173927, 2024 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-38901584

RESUMO

The ubiquity and persistence of organophosphate esters (OPEs) and heavy metal (HMs) pose global environmental risks. This study explored tris(2-chloroisopropyl)phosphate (TCPP) biomineralization coupled to lead (Pb2+) biostabilization driven by denitrifying bacteria (DNB). The domesticated DNB achieved synergistic bioremoval of TCPP and Pb2+ in the batch bioreactor (efficiency: 98 %).TCPP mineralized into PO43- and Cl-, and Pb2+ precipitated with PO43-. The TCPP-degrading/Pb2+-resistant DNB: Achromobacter, Pseudomonas, Citrobacter, and Stenotrophomonas, dominated the bacterial community, and synergized TCPP biomineralization and Pb2+ biostabilization. Metagenomics and metaproteomics revealed TCPP underwent dechlorination, hydrolysis, the TCA cycle-based dissimilation, and assimilation; Pb2+ was detoxified via bioprecipitation, bacterial membrane biosorption, EPS biocomplexation, and efflux out of cells. TCPP, as an initial donor, along with NO3-, as the terminal acceptor, formed a respiratory redox as the primary energy metabolism. Both TCPP and Pb2+ can stimulate phosphatase expression, which established the mutual enhancements between their bioconversions by catalyzing TCPP dephosphorylation and facilitating Pb2+ bioprecipitation. TCPP may alleviate the Pb2+-induced oxidative stress by aiding protein phosphorylation. 80 % of Pb2+ converted into crystalized pyromorphite. These results provide the mechanistic foundations and help develop greener strategies for synergistic bioremediation of OPEs and HMs.


Assuntos
Biodegradação Ambiental , Poluentes Ambientais , Chumbo , Organofosfatos , Organofosfatos/química , Organofosfatos/metabolismo , Retardadores de Chama/metabolismo , Poluentes Ambientais/química , Poluentes Ambientais/metabolismo , Desnitrificação , Chumbo/química , Chumbo/metabolismo , Achromobacter/metabolismo , Pseudomonas/metabolismo , Citrobacter/metabolismo , Stenotrophomonas/metabolismo , Metagenômica , Proteômica , Estresse Oxidativo
14.
J Hazard Mater ; 474: 134624, 2024 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-38810579

RESUMO

Microbiologically induced CaCO3 precipitation (MICP) has been proposed as a potential bioremediation method to immobilize contaminating metals. In this study, carbonate mineralizing bacteria HJ1 and HJ2, isolated from heavy metal contaminated soil, was employed for Cd2+ and Pb2+ immobilization with or without ß-tricalcium phosphate addition. Compared with the only treatments amended with strains, the combined application of ß-tricalcium phosphate and HJ1 improved the immobilization rates of Cd and Pb by 1.49 and 1.70 times at 24 h, and the combined application of ß-tricalcium phosphate and HJ2 increased the immobilization rates of Cd and Pb by 1.25 and 1.79 times. The characterization of biomineralization products revealed that Cd2+ and Pb2+ primarily immobilized from the liquid phase as CdCO3 and PbCO3, and the addition of ß-tricalcium phosphate facilitated the formation of Ca4.03Cd0.97(PO4)3(OH) and Pb3(PO4)2. Also, the calcium source was related to the speciation of carbonate precipitation and improved the Cd and Pb remediation efficiency. This research demonstrated the feasibility and effectiveness of MICP combined with ß-tricalcium phosphate in immobilization of Cd and Pb, which will provide a fundamental basis for future applications of MICP to mitigate soil heavy metal pollutions.


Assuntos
Biodegradação Ambiental , Biomineralização , Cádmio , Fosfatos de Cálcio , Chumbo , Poluentes do Solo , Sporosarcina , Chumbo/metabolismo , Chumbo/química , Fosfatos de Cálcio/química , Fosfatos de Cálcio/metabolismo , Cádmio/metabolismo , Cádmio/química , Sporosarcina/metabolismo , Poluentes do Solo/metabolismo
15.
J Fluoresc ; 2024 May 28.
Artigo em Inglês | MEDLINE | ID: mdl-38805133

RESUMO

The development of luminescent coordination polymers for the selective sensing of Pb2+ in water constitutes an active area of research that impacts analytical, environmental, and inorganic chemistry. Herein, two novel water-stable 2D Zn-coordination polymers {[Zn2(H2O)2(tdc)2(bpy)]·(H2O)}n 1 and [Zn(tdc)(tmb)]n 2 (tdc = thiophenedicarboxylate; bpy = 4,4'-bipyridine and tmb = 4,4'-trimethylenebipyridine) were synthesized, structurally determined by single crystal X-ray diffraction, and studied in-depth as luminescent sensors for a series of cations (Ca2+, Mg2+, Mn2+, Fe2+, Co2+, Ni2+, Cu2+, Zn2+ Cd2+, Hg2+ and Pb2+) in 20% aqueous ethanol. These Zn-polymers possess photostability in 20% aqueous ethanol with a strong emission at 410 upon excitation at 330 nm and quantum yields of around Φ = 0.09. Under these conditions, Pb+2 can be efficiently sensed with polymer 2 through a fluorescent ratiometric response with selectivity over common interfering metal ions such as Cu2+, Cd2+ and Hg2+ in the micromolar concentration range (detection limit = 1.78 ± 10 µM). Such selectivity/affinity of Pb2+ over Hg2+ for luminescent chemosensors is still rare. On the basis of spectroscopic tools (1H NMR, far ATR-IR, PXRD), the X-ray crystal structure of 2, and Scanning Electron Microscopy with Energy-Dispersive X-ray Spectroscopic analysis, the ratiometric fluorescent response is proposed via an efficient metal-ion exchange driven through interactions between thiophenedicarboxylate rings and Pb2+ ions. The use of flexible luminescent Zn-coordination polymers as sensors for selective and direct detection of Pb2+ in aqueous media has been unexplored until now.

16.
BMC Chem ; 18(1): 103, 2024 May 23.
Artigo em Inglês | MEDLINE | ID: mdl-38783370

RESUMO

Fly ash derived from municipal solid waste incinerators (MSWIs) harbors significant quantities of heavy metals with high leaching toxicity, resulting in detrimental environmental effects. Pb2+ in fly ash is the ion most likely to exceed permissible levels. However, chemical stabilization methods demonstrate poor efficacy in stabilizing Pb2+ under acidic conditions. Herein, we have developed a robust acid-resistant chelating polymer (25DTF) for enhanced stabilization of Pb2+ in fly ash. 25DTF was synthesized through the reaction of formaldehyde with 2,5-dithiourea. 25DTF exhibited remarkable chelation efficiency, nearing 100%, for Pb2+ in fly ash. 25DTF demonstrated exceptional chelation efficiency, surpassing 99.9%, when interacting with Pb2+ in fly ash at pH ≤ 7. Even under acidic conditions, 25DTF effectively prevented the secondary dissolution of Pb2+. Additionally, it indicated outstanding Pb2+ chelation efficiency across diverse regions of China. The 25DTF chelating agent shows considerable potential in alleviating metal ion contamination in soil, wastewater, and urban environmental management, thereby fostering advancements in environmental stewardship.

17.
Spectrochim Acta A Mol Biomol Spectrosc ; 317: 124459, 2024 Sep 05.
Artigo em Inglês | MEDLINE | ID: mdl-38749202

RESUMO

A macrocyclic compound, hemicucurbit[6]uril (HemiQ[6]), is employed as the carbon source to produce a novel sort of carbon quantum dots (CQDs) with blue fluorescence in aqueous solution. The CQDs are fully identified by transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), Nuclear Magnetic Resonance (NMR), zeta potential, ultraviolet/visible (UV-vis) and photoluminescence spectroscopy (PL). The nanomaterial is developed for the analysis of Pb2+ in the light of the Resonance Rayleigh scattering (RRS) changes with the increasing Pb2+ concentration. The proposed probe emerges a high selectivity to Pb2+ and excellent sensitivity in the linear concentration range of 0-6 µM with a detection limit low to 0.42 µM, which is superior to the previous values of Pb2+ sensors, as well as the good anti-interference ability is confirmed by the specifical response to Pb2+ in the presence of other metal cations. Therefore, the proposed analysis of Pb2+ is explored for the application in real samples of tap water and lake water, in satisfied results of acceptable recoveries.

18.
Talanta ; 276: 126260, 2024 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-38759364

RESUMO

Lead ion pollution has become a serious public health concern worldwide. Therefore, sensitive detection of Pb2+ is critical to control lead pollution, assess risks, and safeguard the health of vulnerable populations. This study reports a highly sensitive labelling-free electrochemical aptasensor for Pb2+ detection. The aptasensor employs silver-platinum nanoparticles/graphene oxide (AgPt/GO) and Exonuclease III (Exo III) for signal amplification. GO provides high surface area and conductivity for immobilizing AgPt NPs, facilitating the immobilization of aptamer (Apt) probes on the electrode surface. Exo III enzymatically cleaves DNA strands on the electrode surface, releasing DNA segments to amplify the signal further. The synergistic amplification by AgPt/GO and ExoIII enables an extremely wide linear detection range of 0.05 pM-5 nM for Pb2+, with a low detection limit of 0.019 pM. Additionally, the G-quadruplex structure ensures excellent selectivity for Pb2+ detection, resulting in high reproducibility and stability of the aptasensor. The aptasensor was successfully applied to detect spiked Pb2+ in tap water samples, achieving recovery rates ranging from 96 to 108.4 %. By integrating nanomaterials, aptamers and enzymatic amplification, the aptasensor facilitates highly sensitive and selective detection of Pb2+, demonstrating potential for practical applications in environmental monitoring.


Assuntos
Aptâmeros de Nucleotídeos , Técnicas Biossensoriais , Técnicas Eletroquímicas , Exodesoxirribonucleases , Grafite , Chumbo , Nanocompostos , Platina , Prata , Grafite/química , Chumbo/análise , Chumbo/química , Aptâmeros de Nucleotídeos/química , Exodesoxirribonucleases/química , Técnicas Eletroquímicas/métodos , Platina/química , Nanocompostos/química , Prata/química , Técnicas Biossensoriais/métodos , Nanopartículas Metálicas/química , Limite de Detecção , Poluentes Químicos da Água/análise , Água Potável/análise , Eletrodos , Quadruplex G
19.
Mikrochim Acta ; 191(6): 358, 2024 May 31.
Artigo em Inglês | MEDLINE | ID: mdl-38819654

RESUMO

A signal-amplified platform was designed to construct a label-free electrochemical aptasensor for lead ions (Pb2+) assay. First, flower-like molybdenum disulfide-supported AuNPs (AuNPs@MoS2) nanocomposites were synthesized and used as substrates for modifying the electrode. The AuNPs@MoS2 material possessed large surface area and superior biocompatibility, which was beneficial to improve the loading amount of the complementary DNA (cDNA) and amplified the response signal. Importantly, the prepared core-shell Pt@Pd bimetallic nanoparticles (Pt@PdNPs) were used to conjugate with redox marker thionine (Thi) and aptamer (Apt) for further signal amplification; the obtained signal probes (Thi-Pt@PdNPs-Apt) were connected by the cDNA assembled on the electrode through DNA hybridization. Differential pulse voltammetry was performed to monitor the signal of Thi. After incubating of aptasensor with Pb2+, the specific recognition of Pb2+ and Apt resulted in the dissociation of aptamer-cDNA complex, thereby the Thi-Pt@PdNPs-Apt separated from the electrode surface and decreased current response was obtained. The prepared electrochemical sensor exhibited linear response to Pb2+ in the range 5.0 × 10-4-100 nM and a detection limit of 1.0 × 10-4 nM was achieved. The sensor was applied to the determination of Pb2+ in actual sample with high sensitivity and accuracy, demonstrating potential applications in heavy metal monitoring.

20.
Biochimie ; 225: 146-155, 2024 May 29.
Artigo em Inglês | MEDLINE | ID: mdl-38821199

RESUMO

The industrial world exposes living organisms to a variety of metal pollutants. Here we investigated whether such elements affect G-rich sequences susceptible to fold into G-quadruplex (GQ) structures. Thermal stability and conformation of these oligoncleotides was studied at various molar ratios of a variety of heavy metal salts using thermal FRET, transition-FRET (t-FRET) and circular dichroism. Metal ions affected the thermal stability of the GQs to different extents; some metals had no effect on Tm while other metals caused small to moderate changes in Tm at 1:1 or 1:10 molar ratio. While most of the metals had no major effect, Al3+, Cd2+, Pb2+, Hg2+ and Zn2+ altered the thermal stability and structural features of the GQs. Some metals such as Pb2+ and Hg2+ exhibit differential interactions with telomere, c-myc and c-kit GQs. Overall, toxic heavy metals affect G-quadruplex stability in a sequence and topology dependent manner. This study provides new insight into how heavy metal exposure may affect gene expression and cellular responses.

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