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1.
Tob Control ; 32(3): 359-365, 2023 05.
Artigo em Inglês | MEDLINE | ID: mdl-34667104

RESUMO

INTRODUCTION: Raising tobacco prices via increased taxation may be undermined by tobacco industry tactics to keep budget cigarettes on the market. Price differentials between budget and premium cigarettes allow smokers to trade down in the face of average price rises thus attenuating health benefits. This study examines global trends of price differentials and associations with taxation. METHODS: Ecological analysis of country-level panel data of 195 countries' price differentials was performed and compared against total, specific excise, ad valorem and other taxation. Price differentials were expressed as the difference between budget cigarette and premium pack prices (as % of premium pack prices). Two-level linear regression models with repeated measurements (2014, 2016 and 2018) nested within each country assessed the association between country-level taxation structures and price differentials, adjusted for year, geographical region and income group. RESULTS: Worldwide, median price differential between budget and premium 20-cigarette packs was 49.4% (IQR 25.9%-70.0%) in 2014 and 44.4% (IQR 22.5%-69.4%) in 2018 with significant regional variation. The largest price differentials in 2018 were in Africa, with the lowest in Europe. Total taxation was negatively associated with price differentials (-1.5%, 95% CI -2.5% to -0.4% per +10% total taxation) as was specific excise taxation (-2.5%, 95% CI -3.7% to -1.2% per +10% specific excise tax). We found no statistically significant association between ad valorem taxation and price differentials. CONCLUSION: Total levels of taxation and specific excise taxes were associated with smaller price differentials. Implementing high specific excise taxes may reduce price differentials and improve health outcomes.


Assuntos
Indústria do Tabaco , Produtos do Tabaco , Humanos , Fumar , Comércio , Impostos
2.
Anal Bioanal Chem ; 415(3): 447-456, 2023 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-36357598

RESUMO

Establishing an effective signal amplification strategy is the key to achieving sensitive detection of analytes by electrochemical immunoassay. In this work, a novel sandwich-type electrochemical immunosensor with dual-signal amplification was successfully constructed using PtPd/Cu-TCPP(Fe) as the sensing platform and mesoporous silicon dioxide as the signal amplifier. Firstly, two-dimensional wrinkled Cu-TCPP(Fe) nanomaterials loaded with PtPd nanoparticles have strong affinity for the immobilization of capture antibodies and can generate excellent electrochemical signals. Meanwhile, the mesoporous silicon dioxide with large steric hindrance was used as signal label to further improve the sensitivity of the immunosensor by increasing the difference of the current response signal. Under optimal experimental conditions, the electrochemical immunosensor exhibited a wide linear detection range from 0.1 pg/mL to 1.0 µg/mL, with a detection limit as low as 0.166 fg/mL. The experimental results showed that the constructed immunosensor has a great application prospect in clinical biomarker detection.


Assuntos
Técnicas Biossensoriais , Nanopartículas Metálicas , Nanocompostos , Antígeno Carcinoembrionário , Técnicas Biossensoriais/métodos , Anticorpos Imobilizados , Imunoensaio/métodos , Dióxido de Silício , Técnicas Eletroquímicas/métodos , Ouro , Limite de Detecção
3.
ACS Omega ; 8(51): 49218-49227, 2023 Dec 26.
Artigo em Inglês | MEDLINE | ID: mdl-38162785

RESUMO

In this study, a facile and cost-effective hydrothermal synthesis method was used to synthesize zinc oxide nanoflowers modified by reduced graphene oxide, and subsequently, trimetallic AuPtRu nanoparticles(AuPtRuNPs) were supported via the reduction method for high-sensitivity colorimetric detection of H2O2 in weakly acidic solutions. Compared to monometallic and bimetallic nanoparticles, trimetallic nanoparticles exhibit significant synergistic effects and enhanced catalytic activity. After providing a three-dimensional structure with multiple pores by zinc oxide and enhancing electron transfer ability by reduced graphene, the trimetallic nanocomposites (AuPtRu/ZnO-rGO) exhibited excellent peroxidase-mimicking activity, which can effectively catalyze 3,3',5,5'-tetramethylbenzidine (TMB) to produce a blue oxidation product (oxTMB) in the presence of H2O2. Compared to horseradish peroxidase (HRP), AuPtRu/ZnO-rGO demonstrated significantly enhanced catalytic velocity (Vmax = 6.16 × 10-8 M/s) and affinity (Km = 0.02) for H2O2. The study of the catalytic mechanism showed that trimetallic Au, Pt, and Ru could effectively catalyze H2O2 to produce hydroxyl radicals (•OH) to accelerate the oxidation of TMB and enhance the peroxidase-mimicking activity of the AuPtRu/ZnO-rGO nanocomposites. The results showed that the as-synthesized hydrangea-like AuPtRu/ZnO-rGO nanocomposites showed enhanced peroxidase-mimicking activity. It could be used for the colorimetric detection of H2O2 in the range 5-1000 µM with a LOD of 3.0 µM (S/N = 3), and the recoveries are 93.0-101.7%. In addition, the AuPtRu/ZnO-rGO nanocomposites have good applicability for sensitive colorimetric determination of H2O2 in milk, and it has broad application prospects as a multifunctional sensing platform in the food processing industry.

4.
Talanta ; 248: 123605, 2022 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-35671548

RESUMO

In this work, a brief electrochemical aptasensor was developed for highly sensitive detection of SARS-CoV-2 antigen utilizing an aptamer-binding induced multiple hairpin assembly strategy for signal amplification. In the presence of SARS-CoV-2, a pair of aptamers was brought in a close proximity according to the aptamer-protein antigen binding, which initiated strand displacement reaction thereby triggering a multiple hairpin assembly to obtain long linear DNA concatemers on the electrode surface. As the fabricated hairpin probes were labeled with biotin, massive streptavidin-alkaline phosphatases (ST-ALP) could be further introduced on the electrode interface via biotin-streptavidin interaction thus generating strong electrochemical signal in electrolyte solution containing 1-naphthol phosphate. Benefiting from the non-enzymatic multiple hairpin assembly signal amplification strategy, the designed aptasensor for SARS-CoV-2 spike protein detection exhibited the wide linear range from 50 fg·mL-1 to 50 ng·mL-1 and low detection limit of 9.79 fg·mL-1. Meaningfully, this proposed electrochemical assay provided a potential application for the point of care analysis of viral diseases under ambient temperature.


Assuntos
Aptâmeros de Nucleotídeos , Técnicas Biossensoriais , COVID-19 , Aptâmeros de Nucleotídeos/genética , Biotina , COVID-19/diagnóstico , Técnicas Eletroquímicas , Ouro , Humanos , Limite de Detecção , SARS-CoV-2 , Glicoproteína da Espícula de Coronavírus , Estreptavidina
5.
Angew Chem Int Ed Engl ; 61(34): e202207300, 2022 Aug 22.
Artigo em Inglês | MEDLINE | ID: mdl-35761506

RESUMO

To enhance the fluorescence efficiency of semiconductor nanocrystal quantum dots (QDs), strategies via enhancing photo-absorption and eliminating non-radiative relaxation have been proposed. In this study, we demonstrate that fluorescence efficiency of molybdenum disulfide quantum dots (MoS2 QDs) can be enhanced by single-atom metal (Au, Ag, Pt, Cu) modification. Four-fold enhancement of the fluorescence emission of MoS2 QDs is observed with single-atom Au modification. The underlying mechanism is ascribed to the passivation of non-radiative surface states owing to the new defect energy level of Au in the forbidden band that can trap excess electrons in n-type MoS2 , increasing the recombination probability of conduction band electrons with valence band holes of MoS2 . Our results open an avenue for enhancing the fluorescence efficiency of QDs via the modification of atomically dispersed metals, and extend their scopes and potentials in a fundamental way for economic efficiency and stability of single-atom metals.

6.
Anal Chem ; 94(6): 3013-3019, 2022 02 15.
Artigo em Inglês | MEDLINE | ID: mdl-35119821

RESUMO

Despite having the potential to synthesize stable metal-organic frameworks (MOFs), rare earth metal-based MOFs have not been exploited extensively. Owing to the high coordination numbers, the MOFs can generate a suitable coordination environment for various applications. Herein, samarium (Sm)-based MOFs were synthesized with three different organic linkers, namely, trimesic acid (TMA), meso-tetra(4-carboxyphenyl)porphine (TCPP), and 1,3,6,8-tetra(4-carboxylphenyl) pyrene(TBPy) by the solvothermal approach. The morphologies of Sm-TMA MOF, Sm-TCPP MOF, Sm-TBPy MOF were rod-shaped, cubic consisting of stacked 2D layers, and spherical made of small cubic structures, respectively. After the electrochemical properties of the synthesized MOFs were investigated, the MOFs were used to fabricate immunosensors for detection of carcinoembryonic antigen using a label-free signaling strategy. The immunosensors exhibited a wide linear detection range and a lower detection limit. The exhibited reproducibility and selectivity of the immunosensors were within the tolerable limits. The established label-free immunosensor has been successfully applied for detection of carcinoembryonic antigen in human serum samples, demonstrating that the rare earth metal-based MOFs are promising for construction of biosensors for medical diagnosis.


Assuntos
Técnicas Biossensoriais , Neoplasias , Biomarcadores Tumorais , Colo , Técnicas Eletroquímicas , Humanos , Imunoensaio , Limite de Detecção , Reprodutibilidade dos Testes , Samário
7.
J Adv Res ; 29: 191-205, 2021 03.
Artigo em Inglês | MEDLINE | ID: mdl-33842016

RESUMO

Introduction: Environmental stress is both a major force of natural selection and a prime factor affecting crop qualities and yields. The impact of the GRAS [gibberellic acid-insensitive (GAI), repressor of GA1-3 mutant (RGA), and scarecrow (SCR)] family on plant development and the potential to resist environmental stress needs much emphasis. Objectives: This study aims to investigate the evolution, expansion, and adaptive mechanisms of GRASs of important representative plants during polyploidization. Methods: We explored the evolutionary characteristics of GRASs in 15 representative plant species by systematic biological analysis of the genome, transcriptome, metabolite, protein complex map and phenotype. Results: The GRAS family was systematically identified from 15 representative plant species of scientific and agricultural importance. The detection of gene duplication types of GRASs in all species showed that the widespread expansion of GRASs in these species was mainly contributed by polyploidization events. Evolutionary analysis reveals that most species experience independent genome-wide duplication (WGD) events and that interspecies GRAS functions may be broadly conserved. Polyploidy-related Chenopodium quinoa GRASs (CqGRASs) and Arabidopsis thaliana GRASs (AtGRASs) formed robust networks with flavonoid pathways by crosstalk with auxin and photosynthetic pathways. Furthermore, Arabidopsis thaliana population transcriptomes and the 1000 Plants (OneKP) project confirmed that GRASs are components of flavonoid biosynthesis, which enables plants to adapt to the environment by promoting flavonoid accumulation. More importantly, the GRASs of important species that may potentially improve important agronomic traits were mapped through TAIR and RARGE-II publicly available phenotypic data. Determining protein interactions and target genes contributes to determining GRAS functions. Conclusion: The results of this study suggest that polyploidy-related GRASs in multiple species may be a target for improving plant growth, development, and environmental adaptation.


Assuntos
Giberelinas/metabolismo , Reguladores de Crescimento de Plantas/genética , Proteínas de Plantas/genética , Fatores de Transcrição/genética , Adaptação Biológica , Arabidopsis/genética , Arabidopsis/crescimento & desenvolvimento , Chenopodium quinoa/genética , Chenopodium quinoa/crescimento & desenvolvimento , Meio Ambiente , Evolução Molecular , Flavonoides/metabolismo , Duplicação Gênica , Regulação da Expressão Gênica de Plantas , Ácidos Indolacéticos/metabolismo , Fotossíntese/genética , Desenvolvimento Vegetal/genética , Reguladores de Crescimento de Plantas/metabolismo , Proteínas de Plantas/metabolismo , Poliploidia , Seleção Genética/genética , Fatores de Transcrição/metabolismo , Transcriptoma
8.
Spectrochim Acta A Mol Biomol Spectrosc ; 236: 118347, 2020 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-32305837

RESUMO

As is known, Zn2+ plays a vital role in a variety of biological processes but excessive exposure of Zn2+ to human beings can cause toxicity, inducing a series of overt poisoning symptoms and neurodegenerative disorders. Thus, we designed and synthesized two quinoline-derived Schiff-bases HL1 and HL2, and investigated the fluorescence emission responses of these two Schiff-bases to various metal ions. A significant enhancement in fluorescence emission band centered at 450 nm was observed in the ethanolic solution of HL1 with addition of Zn2+, while remarkably lower fluorescence emission enhancement was obtained in the case of HL2 in which one methyl group was introduced to the azomethine carbon. In addition, HL1 showed good selectivity and high sensitivity towards Zn2+ in the existence of other various interfering metal ions, and the reversibility and regeneration of HL1 were also perfect for extending its applications in environmental and biological systems. Therefore, HL1 could be identified as a fluorescent probe for sensing Zn2+ environmentally and biologically.


Assuntos
Corantes Fluorescentes/química , Zinco/análise , Compostos Azo/química , Corantes Fluorescentes/síntese química , Limite de Detecção , Espectroscopia de Ressonância Magnética , Quinolinas/química , Bases de Schiff , Sensibilidade e Especificidade , Solventes/química , Espectrometria de Fluorescência , Espectrofotometria Ultravioleta , Tiossemicarbazonas/química , Zinco/química
9.
Biosens Bioelectron ; 143: 111609, 2019 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-31476597

RESUMO

In this research, a sensitive and specific electrochemical biosensor for DNA detection was constructed. The highly sensitivity of this biosensor is due to the exploitation of exonuclease III-assisted double recycling and toehold-mediated strand displacement recycling to achieve the target triple recycling amplification, thus generating a large amount of Y-shaped DNA structures. Combination with a terminal deoxynucleotidyl transferase (TDT)-mediated cascaded signal amplification strategy can catalyze the repetitive incorporation of biotin-dUTP to the 3'-OH of the Y-shaped DNA. Via biotin-streptavidin interaction, multiple streptavidin-alkaline phosphatases were conjugated to the surface of an Au electrode and generated a sharply increasing electrochemical signal in a 1-naphthyl phosphate (1-NP) solution. In this method, an impressive detection limit of 0.05 fM was obtained, presenting outstanding selectivity with a dynamic response scope between 0.1 fM and 1 nΜ. Thus, the designed biosensor opens an avenue for DNA detection in clinical molecular diagnostics, pathogen detection, gene therapy, food safety and environmental monitoring.


Assuntos
Técnicas Biossensoriais , DNA Nucleotidilexotransferase/química , DNA/isolamento & purificação , Técnicas Eletroquímicas , Fosfatase Alcalina/química , Biotina/química , Catálise , DNA/química , Eletrodos , Exodesoxirribonucleases/química , Limite de Detecção , Técnicas de Amplificação de Ácido Nucleico , Estreptavidina/química
10.
Biosens Bioelectron ; 144: 111560, 2019 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-31494504

RESUMO

In this work, a novel Pb2+ electrochemical DNAzyme sensor was developed for ultrasensitive detection of lead ions (Pb2+) in water environment by coupling with the MoS2-AuPt nanomaterials and hemin/G-quadruplex DNAzyme, which acting as the electrocatalytic signal tag. Streptavidin (SA) modified tin dioxide-functionalized reduced graphene oxide (rGO-SnO2) /gold nanoparticles (AuNPs) served as a sensor platform for enhancing conductivity and immobilizing more Pb2+-specific DNAzyme. In the presence of Pb2+, the Pb2+-dependent DNAzyme specifically reacted with Pb2+, cleaving the substrate strand (SS) into two free fragment and releasing the biotin-modified enzyme strand (Bio-ES) on the electrode. Connecting MoS2-AuPt nanocomposites labeled with G-rich DNA (G-DNA) strand and exposure of Bio-ES through the Helper DNA, as well as adding hemin to form a hemin/G-quadruplex, the biosensor achieved signal amplification. Chronoamperometry was used to record the current signal, which was primarily derived from the cocatalysis reduction of H2O2 by MoS2-AuPt nanocomposites and the hemin/G-quadruplex. Under optimal conditions, the designed biosensor exhibited sensitive detection of Pb2+ from 0.1 pg mL-1 to 1000 ng mL-1, with a lower detection limit of 38 fg mL-1 (based on 3σ). This proposed biosensor is ultrasensitive and specific, representing a potential application for the detection of Pb2+ in a water environment.


Assuntos
Técnicas Biossensoriais , DNA Catalítico/química , Técnicas Eletroquímicas , Chumbo/isolamento & purificação , Dissulfetos/química , Quadruplex G , Grafite/química , Hemina/química , Chumbo/química , Nanopartículas Metálicas/química , Molibdênio/química , Paládio/química , Estreptavidina
11.
Phys Chem Chem Phys ; 21(22): 11883-11891, 2019 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-31123740

RESUMO

Early diagnosis of diseases by contrast-enhanced magnetic resonance imaging (MRI) using iron oxide superparamagnetic nanoparticles (IOSNPs) has been extensively investigated due to the good biocompatibility of modified IOSNPs. However, the low magnetic sensitivity of IOSNPs still inflicts a certain limitation on their further application. In this study, we employed first-principles calculations based on spin-polarized density functional theory (SDFT) to find the optimal dysprosium-doped scheme for improving the magnetic sensitivity of IOSNPs. Elicited from the optimal doping scheme, we synthesized a sort of ultrasmall γ-iron oxide superparamagnetic nanoparticle by a special phase transfer-coprecipitation method. The appropriately Dy-doped γ-IOSNPs coated with short-chain polyethylene glycol are small in hydrodynamic size and highly dispersed with effectively improved superparamagnetism for enhancing T2-weighted MRI relaxivity, which is well consistent with the SDFT prediction. The measured spin-spin relaxivity r2 is 123.2 s-1 mM-1, nearly double that of the pure γ-IOSNPs (67.8 s-1 mM-1) and substantially surpassing that of both clinically-approved T2 contrast agents Feridex and Resivist. The low dysprosium doping does not induce notable nanotoxicity for IOSNPs, but contributes sufficiently to their high relaxation performance instead, which endows the Dy-doped γ-IOSNPs with high potential as a better T2-weighted MRI contrast medium. Both the method and the nanomagnets reported in this study are expected to promote studies on designing and preparing high-performance MRI contrast agents as well as computational materials.

12.
Spectrochim Acta A Mol Biomol Spectrosc ; 218: 342-347, 2019 Jul 05.
Artigo em Inglês | MEDLINE | ID: mdl-31026711

RESUMO

Upon excitation of the visible light, probes show colorimetric and fluorescent responses to the specific metal ion, which can be easily detected by the naked eye. Owing to the excitation of the visible light at 423 nm, a novel and simple Schiff-base receptor based chromone derivative called 7-methoxychromone-3-carbaldehyde-(indole-3-formyl) hydrazone (MCIH2) had been investigated as a selective and sensitive probe for Al3+ with colorimetric and fluorescent responses. Upon addition of Al3+ to compound MCIH2 solution, compound MCIH2 could respond to Al3+ with a good selective colorimetric signal, which was easily observed from colorless to yellow-green by the naked eye. Furthermore, a remarkable fluorescence emission enhancement with an "OFF-ON" signal by over 700-fold was triggered, but other various metal ions had no such significant effects on the fluorescence emission. In addition, the detection limit of compound MCIH2 for recognizing Al3+ was evaluated to be as low as 1 × 10-7 M level, which was sufficiently low for sensing Al3+ widely distributed in various environmental and biological systems.

13.
Spectrochim Acta A Mol Biomol Spectrosc ; 204: 641-647, 2018 Nov 05.
Artigo em Inglês | MEDLINE | ID: mdl-29982154

RESUMO

In this study, a novel fluorescent probe, 6­hydroxychromone­3­carbaldehyde­(rhodamine B carbonyl) hydrazine (L), for Zn2+ and Al3+ was designed and synthesized. Initially, this probe L exhibited inferior fluorescence emission peak centered at 488 nm in EtOH/HEPES solution (3/1, 10.0 µM HEPES, pH 7.4) when excited at 421 nm. After the addition of Zn2+, this probe L displayed excellent selectivity towards Zn2+ with obvious fluorescence color change from colorless to yellow, which might be attributed to the formation of a 1:1 ligand-metal complex resulting in the inhibition of photo-induced electron transfer phenomenon. Whereas, the prepared Zn2+ complex of L could be used as a ratiometric fluorescent probe to detect Al3+ on the basis of fluorescence resonance energy transfer mechanism. This ligand-metal complex of Zn2+ (LZn) showed high selectivity towards Al3+ with obvious enhancement in fluorescence emission intensity at 580 nm and remarkable decrease in fluorescence emission intensity at 488 nm, and the fluorescence color also changed from yellow to pink. Furthermore, the detection limit of the probe L, LZn towards Zn2+, Al3+ were 1.25 × 10-7 M and 3.179 × 10-6 M, respectively. Additionally, the complexation properties of L towards Zn2+ and LZn towards Al3+ were studied in detail.

14.
Biosens Bioelectron ; 113: 148-156, 2018 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-29772383

RESUMO

In this work, hollow nanobox metal-organic framework (HNM) nanocomposites were synthesised and utilised for the first time in a signal decreased electrochemical immunosensor for the ultrasensitive quantitative determination of lymphocyte activation gene-3 (LAG-3) protein, which is a newly discovered biomarker. With the aid of signal materials, namely, SiO2-tagged anti-LAG-3 antibody (SiO2-Ab2) and the biotin-streptavidin system, the sensor can achieve signal amplification. Encapsulation of tin dioxide-functionalised reduced graphene oxide (rGO-SnO2) and gold and platinum alloys (AuPt alloys) onto the surface of hollow nanobox metal-organic frameworks (MOFs) was performed to prepare rGO-SnO2/hollow nanobox-MOFs/AuPt alloys (rGO-SnO2/HNMs/AuPt) as the matrix. SiO2-Ab2, which is used as the signal-decreased label, can be utilised to enhance the distinction of the electrochemical signal after the specific recognition between antibodies and antigens, owing to its large steric hindrance property. In this sensor, this proposed sandwich immunosensor can achieve a high sensitivity, especially in the presence of low concentrations of the LAG-3 protein. Under optimal conditions, this sandwich-designed immunosensor exhibited a sensitive detection of the LAG-3 protein from concentrations of 0.01 ng mL-1 to 1 µg mL-1, with a lower detection limit of 1.1 pg mL-1 (based on 3σ). We proposed that this ultrasensitive biosensor can be utilised for the detection of the LAG-3 protein in early clinical tumour diagnosis.


Assuntos
Anticorpos Imobilizados/química , Antígenos CD/sangue , Ouro/química , Grafite/química , Imunoensaio/métodos , Nanoestruturas/química , Platina/química , Ligas/química , Técnicas Biossensoriais/métodos , Biotina/química , Técnicas Eletroquímicas/métodos , Humanos , Limite de Detecção , Nanoestruturas/ultraestrutura , Óxidos/química , Estreptavidina/química , Proteína do Gene 3 de Ativação de Linfócitos
15.
Nanoscale ; 10(18): 8667-8676, 2018 May 10.
Artigo em Inglês | MEDLINE | ID: mdl-29700546

RESUMO

It is well-known that ClO- and SCN- can cause adverse effects on the environment and organisms; therefore, development of new strategies for detecting ClO- and SCN-, especially in water, are highly desirable. Here, we present luminous Eu(iii) complex-functionalized Fe3O4 nanoparticles encapsulated into zeolitic imidazolate framework materials (nano-ZIF-8) and successfully employ this nano-MOF as a fluorescence probe for selective and sensitive detection of ClO- and SCN-. The introduction of ClO- into nano-ZIF-8 solution induced a significant decrease in the characteristic fluorescence emission of Eu3+ at 613 nm. However, strong fluorescence emission was again observed when SCN- was successively injected into the prepared nano-ZIF-8-ClO-. Thus, a novel fluorescence system for simultaneous detection of free ClO- and SCN- was established. On the basis of the superior adsorption performance of nano-MOF materials, free residual ClO- and SCN- in water was rapidly, sensitively and selectively detected with a detection limit of 0.133 nM and 0.204 nM, respectively. Moreover, nano-ZIF-8 was successfully used for monitoring the concentration levels of ClO- and SCN- in specimens of tap water and Yellow River water. Furthermore, the reversibility and regeneration of nano-ZIF-8 in sensing ClO- and SCN- is advantageous for applications of nano-ZIF-8 in solid-state sensing and anti-counterfeiting. As far as we know, this is the first time that nano-MOFs have been used as a selective fluorescence probe for ClO-/SCN- detection and anti-counterfeiting.

16.
Phys Chem Chem Phys ; 20(15): 10038-10047, 2018 Apr 18.
Artigo em Inglês | MEDLINE | ID: mdl-29620132

RESUMO

Gadolinium oxide-based core-shelled nanoparticles have recently emerged as novel magnetic resonance imaging contrast agents for high relaxivity and tumor targeting. However, their relaxivity enhancement mechanism has not yet been clearly understood. We prepared highly dispersible and uniform core-shell structured nanoparticles by encapsulating silica spheres (90 nm in diameter) with gadolinium oxide shells of different thicknesses (from 1.5 nm to 20 nm), and proved experimentally that the shell thickness has an inverse effect on relaxivity. The core-shelled nanoparticles are of a larger relaxivity than the commercial contrast agent Gd-DTPA, with an enhancement from 1.8 to 7.3 times. Based on the Solomon-Bloembergen-Morgan theory which is usually adopted for interpreting the relaxation changes of water protons in Gd3+ chelates, we introduced a shielding ansatz of nanoshells and derived a concise formula specifically to correlate the relaxivity of this sort of core-shelled nanoparticles with the shell thickness directly. The formula calculation is well consistent with the experimental results, and the formula can be generally applied to evaluate the relaxation enhancement underlying the high relaxivity of any core-shelled nanoparticle. Furthermore, the core-shelled nanoparticles possess a negligible nanotoxicity according to the in vitro cytotoxicity and in vivo histopathology and hematology assays. The enhanced signals of in vivo tumor-targeted magnetic resonance imaging indicate that the ultrathin gadolinium oxide nanoshells may function as a potential candidate for advanced positive contrast agents in further clinical applications.

17.
Biosens Bioelectron ; 99: 338-345, 2018 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-28800505

RESUMO

In this work, novel octahedral Cu2O-Au nanocomposites were synthesized and first applied in an electrochemical aptasensor to detect thrombin (TB) with the aid of a DNAzyme for signal amplification. The octahedral Cu2O-Au nanocomposites have not only simultaneously served as signal amplifying molecules but have also been utilized as an ideal loading platform to immobilize a large number of electroactive substances and recognition probes. Gold nanoparticles (AuNPs) were grown directly on the surface of the octahedral Cu2O nanocrystals, and the Cu2O-Au nanocomposites obtained had the advantages of large surface areas and excellent biocompatibilities. The hemin/G-quadruplex, which was formed by intercalating hemin into the amino terminated thrombin binding aptamer (NH2-TBA), and the electroactive toluidine blue (Tb) were immobilized onto the Cu2O-Au nanocomposite surfaces through a stable Au-N bond. AuNPs, Cu2O and hemin/G-quadruplex co-catalyse the H2O2 in the working buffer to promote the electron transfer of Tb as a multiple signal amplification strategy in order to improve the performance of the electrochemical aptasensor. Under optimal conditions, the designed aptasensor exhibited sensitive detection of TB from 100 fM to 20nM with a lower detection limit of 23fM. This proposed aptasensor exhibited good sensitivity, high specificity and acceptable reproducibility and could be widely applied in bioassay analysis.


Assuntos
Aptâmeros de Nucleotídeos/química , Técnicas Biossensoriais , DNA Catalítico/química , Trombina/isolamento & purificação , Catálise , Cobre/química , Técnicas Eletroquímicas , Quadruplex G , Hemina/química , Humanos , Limite de Detecção , Nanopartículas Metálicas/química , Nanocompostos/química , Trombina/química
18.
Spectrochim Acta A Mol Biomol Spectrosc ; 193: 415-421, 2018 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-29277072

RESUMO

In this paper, a simple naphthalene-based derivative (HL) has been designed and synthesized as a Al3+-selective fluorescent chemosensor based on the PET mechanism. HL exhibited high selectivity and sensitivity towards Al3+ over other commonly coexisting metal ions in ethanol with a detection limit of 2.72nM. The 1:1 binding stoichiometry of the complex (HL-Al3+) was determined from the Job's plot based on fluorescence titrations and the ESI-MS spectrum data. Moreover, the binding site of HL with Al3+ was assured by the 1H NMR titration experiment. The binding constant (Ka) of the complex (HL-Al3+) was calculated to be 5.06×104M-1 according to the Benesi-Hildebrand equation. In addition, the recognizing process of HL towards Al3+ was chemically reversible by adding Na2EDTA. Importantly, HL could directly and rapidly detect aluminum ion through the filter paper without resorting to additional instrumental analysis.

19.
Nanoscale ; 9(43): 16661-16673, 2017 Nov 09.
Artigo em Inglês | MEDLINE | ID: mdl-28809413

RESUMO

Multifunctional nanoprobes, due to their unique nanocomposite structures, have prominent advantages that combine multimodal imaging of a tumor with photothermal therapy. However, they remain a challenge for constructing nanostructures via conventional approaches due to the peculiar environmental sensitivity of each component. Here, we report the design and synthesis of Gd-based nanoparticle-tailored gold nanorods with distinctive core-shell and dumbbell nanoarchitectures (NAs) by a specific synthesis technology. The prepared NAs possess a tunable particle size of 80-120 nm in length and 50-90 nm in diameter, which are suitable for cellular uptake and passive targeting of a tumor. The formation of two distinct heterostructures and their underlying mechanism were studied through systematic investigations on the controllable synthesis process. The as-prepared nanoprobes possess an ultrahigh longitudinal relaxivity (r1) of 22.69 s-1 mM-1 and thus a significant magnetic resonance imaging signal enhancement has been observed in mice tumors. The NAs, especially the dumbbell type, show a vivid two-photon cell imaging and a remarkable photothermal conversion efficiency owing to their superior longitudinal surface plasmon resonance. Both in vitro cytotoxicity and in vivo immunotoxicity assays give substantial evidence of excellent biocompatibility attained in the NAs. The development of multifunctional targeting nanoprobes in this study could provide guidance for tailored design and controllable synthesis of heterostructured nanocomposites utilized for multimodal imaging and photothermal therapy of cancer.

20.
Phys Chem Chem Phys ; 19(7): 5366-5376, 2017 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-28155924

RESUMO

We report a class of multi-functional core-shell nanoarchitectures, consisting of silica nanospheres as the core and Gd2O3:Dy3+ nanocrystals as the ultra-thin shell, that enable unique multi-color living cell imaging and remarkable in vivo magnetic resonance imaging. These types of targeted cell imaging nanoarchitectures can be used as a variety of fluorescence nanoprobes due to the multi-color emissions of the Gd2O3:Dy3+ nanophosphor. We also proposed a strategy of modulating core-shell structure design to achieve an enhanced magnetic resonance contrast ability of Gd2O3 nanoagents, and the classical Solomon-Bloembergen-Morgan theory was applied to explicate the mechanism underlying the enhancement. The as-synthesized ligand-free nanomaterial possesses a suitable particle size for cellular uptake as well as avoiding penetrating the blood-brain barrier with good water-solubility, stability, dispersibility and uniformity. The extremely low cytotoxicity and favorable biocompatibility obtained from in vitro and in vivo bioassays of the as-designed nanoparticles indicate their excellent potential as a candidate for functioning as a targeted nanoprobe.


Assuntos
Disprósio/química , Corantes Fluorescentes/química , Corantes Fluorescentes/toxicidade , Gadolínio/química , Imageamento por Ressonância Magnética , Nanopartículas/química , Imagem Óptica , Animais , Sobrevivência Celular/efeitos dos fármacos , Gadolínio/toxicidade , Células HEK293 , Células HeLa , Humanos , Camundongos , Nanopartículas/toxicidade
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