Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 125
Filtrar
1.
Anal Chem ; 96(22): 9026-9033, 2024 Jun 04.
Artigo em Inglês | MEDLINE | ID: mdl-38771095

RESUMO

Precise detection of a trace substance that intrinsically possesses weak chemical activity and less-distinctive spatial structure is of great significance, but full of challenges, as it could not be effectively recognized via either an active covalent reaction process or multiple noncovalent interactions toward its simple structure. Here, the electronic-effect-driven recognition strategy was proposed to visually sense an illicit drug, γ-hydroxybutyric acid (GHB), which was treated as an analyte model due to its inherent simple structure. In particular, a sensing system composed of two probes substituted by the nitro (-NO2) and the hydrogen (-H), was constructed with the characteristic yellow coloring and blue fluorescence, as well as high sensitivity (0.586 ng/mL), fast response (0.2 s), and specific recognition, even in the presence of 22 interferents. In addition, a portable eyeshadow box-like sensing chip was fabricated and proven to be reliable and feasible in sensing GHB disguised in liquors for self-protection in a covert manner. Hence, this work developed an electronic-effect-driven modulation strategy of the recognition interaction between the probe and the analyte and, thus, would open up a new thought for detecting the analyte with weak activity and a simple structure, as well as propel the relevant application in real scenarios.

2.
Inorg Chem ; 63(19): 8889-8898, 2024 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-38693871

RESUMO

Phosphor-in-glass represents a promising avenue for merging the luminous efficiency of high-quality phosphor and the thermal stability of a glass matrix. Undoubtedly, the glass matrix system and its preparation are pivotal factors in achieving high stability and preserving the original performance of embedded phosphor particles. In contrast to the well-established commercial Y3Al5O12:Ce3+ oxide phosphor, red nitride phosphor, which plays a critical role in high-quality lighting, exhibits greater structural instability during the high-temperature synthesis of inorganic glasses. A telluride glass with a refractive index (RI = 2.15@615 nm) akin to that of nitride phosphor (∼2.19) has been devised, demonstrating high efficiency in photon utilization. The lower glass-transition temperature plays a crucial role in safeguarding phosphor particles against erosion resulting from exposure to high-temperature melts. Phosphor-in-glass retains 93% of the quantum efficiency observed for pure phosphor. The assembled white light-emitting diodes module has precise color tuning capabilities, achieving an optimal color rendering index of 93.7, a luminous efficacy of 80.4 lm/W, and a correlated color temperature of 5850 K. These outcomes hold potential for advancing the realm of inorganic package and high-quality white light illumination.

3.
J Phys Chem A ; 128(18): 3571-3578, 2024 May 09.
Artigo em Inglês | MEDLINE | ID: mdl-38656182

RESUMO

It is of great importance to understand the intrinsic relationship between phototautomerization and photoelectric properties for the exploration of novel organic materials. Here, in order to chemically control the protonation process, the aminated isoxazole derivative (2,2'-(isoxazolo[5,4-d]isoxazole-3,6-diyl)dibenzenaminium, DP-DA-DPIxz) with -N═ as the proton acceptor was designed to achieve the twisted intramolecular charge transfer (TICT) state which was triggered by an excited-state intramolecular proton transfer (ESIPT) process. This kind of protonation enhanced the intramolecular hydrogen bonding, conjugative effect, and steric hindrance effects, ensuring a barrierless spontaneous TICT process. Through the intramolecular proton transfer, the configuration torsion and conjugation dissociation of the DP-DA-DPIxz molecule was favored, which led to efficient charge separation and remarkable variations in light-emitting properties. We hope the present investigation will provide a new approach to design novel optoelectronic organic materials and shine light on the understanding of the charge transfer and separation process in molecular science.

4.
Angew Chem Int Ed Engl ; 63(15): e202400453, 2024 Apr 08.
Artigo em Inglês | MEDLINE | ID: mdl-38323751

RESUMO

Aggregation-induced emission (AIE) shows promising performance in chemical sensing relying on the change of the emission behavior of the probe molecule monomers to the aggregated product. However, whether the response contrast could be further boosted by utilizing the emission property of the aggregated probe and the aggregated product remains a big challenge. Here, an exciting AIE probe regulation strategy was proposed by coherently modulating the aggregation behavior and the intramolecular charge transfer (ICT) property of the probes and thus an aggregated-to-aggregated colorimetric-fluorescent dual-mode detection was achieved. The blue emissive film obtained with the optimal AIE probe has been proven to be effective to recognize the vapor of nerve agent analog DCP in air by emitting a sharp green fluorescence. In addition, a porous polymer-based wet sensing chip loaded with the probe enables the immediate response to DCP vapor with a limit of detection (LOD) of 1.7 ppb, and it was further integrated into a wearable watch device for long-term monitoring of DCP vapor up to two weeks. We expect the present probe design strategy would greatly deepen the AIE-based science and provide new insights for long-term monitoring sensors toward trace hazardous substances.


Assuntos
Corantes Fluorescentes , Agentes Neurotóxicos , Corantes Fluorescentes/química , Espectrometria de Fluorescência , Colorimetria
5.
Org Biomol Chem ; 21(2): 315-322, 2023 01 04.
Artigo em Inglês | MEDLINE | ID: mdl-36524697

RESUMO

A deep understanding of the fluorescence response mechanisms is the foundation for design-oriented strategies for D-π-A probes for trace hazardous chemicals. Here, from the perspective of electronegativity regulation of the π-bridge recognition site, an electron-donation modulation strategy involving various comprehensive evaluations of the optical and chemical properties is proposed through a series of theoretical analyses. Due to the preferential combined interaction between the π-bridge recognition site and MnO4-, high electrophilic reactivity and feasible chemical reaction energy barrier, a high-performance filter paper chip and hydrogel chip for the detection of aqueous and air-suspended environmental KMnO4 was achieved. We expect the present modulation strategy will facilitate efficient fluorescent probe design and provide a universal methodology for the exploration of functional D-π-A molecules.


Assuntos
Elétrons , Corantes Fluorescentes , Corantes Fluorescentes/química , Teoria da Densidade Funcional , Fluorescência
6.
J Phys Chem A ; 127(4): 902-912, 2023 Feb 02.
Artigo em Inglês | MEDLINE | ID: mdl-36669096

RESUMO

The exploration of the intrinsic relationship between the phototautomerization and photoelectric properties is of great significance for the application of the emerging novel organic materials, such as the (bi)heterocyclic thiazolo[5,4-d]thiazole derivatives (TzTz). Here, by introducing the chemical-controlling protonation, a barrierless spontaneous rotation movement of the designed TzTz derivative (2,5-diyl-amino-thiazolo[5,4-d]thiazole, DA-TzTz) was ensured through the facilitation of the excited-state intramolecular proton transfer (ESIPT) triggered twisted intramolecular charge transfer (TICT) process by the enhancement of the intramolecular hydrogen bonds, steric hindrance effect, and conjugative effect. It is further verified that the hetero S atoms could mostly effect the proton accepting ability of -N═ through comparing with the influences to the intramolecular H-bond between the protonated/nonprotonated amino groups and the -N═ atoms brought by the replacement of them with N or O atoms. As a result, the dissociation and rearrangement of the π conjugation in DA-TzTz accompanying with the variation of the optoelectronic characteristics was benefited from the establishment of the preferential charge-transfer and separation. We expect this tentative study could establish a new concept of designing an efficient charge-transfer and separation method, paving the way for the development of the TzTz derivatives and other optoelectronic organic materials.

7.
J Environ Sci (China) ; 125: 194-204, 2023 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-36375905

RESUMO

Sb(III) is often detected in contaminated soil and groundwater. Hence, high-efficiency technology is needed. In this study, bimetallic organic frameworks were used for the first time to immobilize Sb(III) from contaminated soil and groundwater. The materials were synthesized by the hydrothermal method. Both ends of the prepared material were hexagonal tip rods, and the length became shorter as the ratio of Fe/Mg decreased. The bimetallic organic framework with a Fe/Mg feeding ratio of 0.5 was the optimum material for Sb(III) removal, which could effectively immobilize Sb(III). The adsorption isotherm was fitted well with the Freundlich model, and the optimal adsorption capacity can reach 106.97 mg/g. The adsorption capacity of 84% can be completed in 10 min, which conformed to the pseudo-second-order kinetics. The Fe3+ could enhance the stability of the material, and the Mg2+ was conducive to freeing up adsorption sites for binding Sb(III) and forming stable chemical adsorption. Ion exchange is the predominant mechanism to remove Sb(III). After 14 days of remediation of Sb(III) contaminated soil, the Toxicity Characteristic Leaching Procedure (TCLP)-leached concentrations of Sb(III) were reduced by 86%, 91% and 94% when the material dosages were 1%, 2% and 3%, respectively. Immobilization of Sb(III) in soil resulted in a conversion of antimony speciation from more easily bioavailable species to less bioavailable species, further contributing to reduce the environmental risk of antimony. The results indicate that ferro-magnesium bimetallic organic frameworks may serve as a kind of promising materials for the immobilization of Sb(III) in contaminated soil and groundwater.


Assuntos
Água Subterrânea , Poluentes do Solo , Antimônio/análise , Solo , Magnésio , Poluentes do Solo/análise , Adsorção
8.
Am J Hum Genet ; 105(6): 1102-1111, 2019 12 05.
Artigo em Inglês | MEDLINE | ID: mdl-31679651

RESUMO

Recurrent miscarriage (RM) affects millions of couples globally, and half of them have no demonstrated etiology. Genome sequencing (GS) is an enhanced and novel cytogenetic tool to define the contribution of chromosomal abnormalities in human diseases. In this study we evaluated its utility in RM-affected couples. We performed low-pass GS retrospectively for 1,090 RM-affected couples, all of whom had routine chromosome analysis. A customized sequencing and interpretation pipeline was developed to identify chromosomal rearrangements and deletions/duplications with confirmation by fluorescence in situ hybridization, chromosomal microarray analysis, and PCR studies. Low-pass GS yielded results in 1,077 of 1,090 couples (98.8%) and detected 127 chromosomal abnormalities in 11.7% (126/1,077) of couples; both members of one couple were identified with inversions. Of the 126 couples, 39.7% (50/126) had received former diagnostic results by karyotyping characteristic of normal human male or female karyotypes. Low-pass GS revealed additional chromosomal abnormalities in 50 (4.0%) couples, including eight with balanced translocations and 42 inversions. Follow-up studies of these couples showed a higher miscarriage/fetal-anomaly rate of 5/10 (50%) compared to 21/93 (22.6%) in couples with normal GS, resulting in a relative risk of 2.2 (95% confidence interval, 1.1 to 4.6). In these couples, this protocol significantly increased the diagnostic yield of chromosomal abnormalities per couple (11.7%) in comparison to chromosome analysis (8.0%, chi-square test p = 0.000751). In summary, low-pass GS identified underlying chromosomal aberrations in 1 in 9 RM-affected couples, enabling identification of a subgroup of couples with increased risk of subsequent miscarriage who would benefit from a personalized intervention.


Assuntos
Aborto Habitual/diagnóstico , Aborto Habitual/genética , Aberrações Cromossômicas , Sequenciamento Completo do Genoma/métodos , Adulto , Feminino , Seguimentos , Humanos , Cariotipagem , Masculino , Gravidez , Prognóstico , Estudos Retrospectivos
9.
Anal Chem ; 94(16): 6318-6328, 2022 04 26.
Artigo em Inglês | MEDLINE | ID: mdl-35427131

RESUMO

Achieving sensitive and robust colorimetry is of great significance for on-site chemical detection, but has always been a dilemma or at the expense of practicality. Here, from the perspective of solvent, which is commonly the indispensable medium for chemical sensing, the solvent induction strategy concerning the hydrophobic shielding and hydrophilic bonding solvent cage was proposed considering the configuration branching ratio in the reagent and the prevention of the autoxidation channel. Due to the competitive delocalized charge transfer in the probe and the effective viscous drag in the reagent, remarkable sensing signal concentrating and moisture retention capability were achieved. We expect the present strategy would facilitate the active but robust chemical reaction design and provide a universal methodology for the exploration of high-performance chemical sensors.


Assuntos
Colorimetria , Ureia , Colorimetria/métodos , Solventes
10.
Anal Chem ; 94(33): 11679-11687, 2022 08 23.
Artigo em Inglês | MEDLINE | ID: mdl-35948453

RESUMO

Inhibition of twisting intramolecular charge transfer (TICT) is one of the most attractive methods for fluorescence-on analysis, whereas it remains enigmatic whether the fluorescence in a TICT-based probe could be thoroughly lightened. Here, for maximizing the fluorescence-on signal of the TICT-based probe, we develop a model by employing chemical reaction to directly cleave the linkage between the rotational electron donor and acceptor with a predisposed fluorescent signal close to zero. To validate this assumption, a nonfluorescent probe with barrierless rotation is successfully achieved by grafting acryloyl with -C═C- recognition sites onto coumarin, and 7-hydroxycoumarin with bright blue fluorescence could be released within 3 s upon probing KMnO4 with an amount as low as 0.95 nM and 6.6 pg. We believe that the present strategy could not only deepen the insights of photochemistry but also facilitate the development of a theranostic drug delivery system, energy conversion, pollution control, and health risk reduction.


Assuntos
Corantes , Fluorescência , Fotoquímica , Rotação
11.
Anal Chem ; 94(41): 14322-14330, 2022 Oct 18.
Artigo em Inglês | MEDLINE | ID: mdl-36208485

RESUMO

Semiconducting polymer has a high extinction coefficient and a long band absorption and can be used as a photoacoustic imaging contrast agent. However, nonbiodegradable semiconducting polymers may cause biosafety issues due to being retained in the body. Therefore, developing degradable semiconducting polymers is necessary for in vivo imaging. Herein, we developed three degradable semiconducting polymers with unique optical properties. We adjusted the optical properties of semiconducting polymers by designing the molecular structure of semiconducting polymers. Polymers with a donor-π-acceptor structure could easily improve the optical properties through adjusting the donor or acceptor units. Through adjusting the electron-donor and -acceptor units, three diketopyrrolopyrrole derivative polymers (DPPTz, DPPQu, and DPPWu) were synthesized and converted into nanosize particles. By introducing the degradable chemical groups in the main chain structure of semiconducting polymers, diketopyrrolopyrrole polymers could be degraded by ClO-. Among these nanosize particles, DPPTz NPs and DPPQu NPs were used to achieve the in vivo photoacoustic imaging of λ-carrageenan-induced arthritis mouse model. This work provides a novel design idea for the designing of red-shifted semiconducting polymer with degradable properties.


Assuntos
Artrite , Nanopartículas , Técnicas Fotoacústicas , Animais , Carragenina , Meios de Contraste , Modelos Animais de Doenças , Cetonas , Camundongos , Nanopartículas/química , Técnicas Fotoacústicas/métodos , Polímeros/química , Pirróis , Espectroscopia de Luz Próxima ao Infravermelho/métodos
12.
Arch Microbiol ; 204(6): 299, 2022 May 06.
Artigo em Inglês | MEDLINE | ID: mdl-35513559

RESUMO

Microbiologically influenced corrosion (MIC) is becoming a knotty problem for transmission pipelines. Developing MIC mitigation strategies for pipelines is increasingly urgent. In this study, MIC resistance against Pseudomonas aeruginosa of the X65 pipeline steels with (X65Cu) and without (X65) Cu addition was comparatively studied by electrochemical measurements and surface observation. Experimental results demonstrated that the corrosion rate of X65Cu steel was lower than that of X65 steel no matter in sterile or bacteria-containing media. Cu addition is helpful to the formation of the rust layer in the sterile medium. Surface observation showed that X65Cu steel exhibited a better MIC resistance against P. aeruginosa than that of X65 steel. Cu ions released from the X65Cu steel could effectively kill the P. aeruginosa attached on the steel surface, thus evidently decreased the pit depth and diameter.


Assuntos
Pseudomonas aeruginosa , Aço , Biofilmes , Corrosão , Aço/farmacologia
13.
Inorg Chem ; 61(38): 15116-15129, 2022 Sep 26.
Artigo em Inglês | MEDLINE | ID: mdl-36094380

RESUMO

NH4Ln(MoO4)2 (Ln = La-Lu lanthanide, Y) was crystallized via hydrothermal reaction as a new family of layered materials, from which phase-pure Ln2Mo4O15 was successfully derived via subsequent annealing at 700 °C for the series of Ln elements excluding Ce and Lu. Detailed structure analysis revealed that the ionic size of Ln3+ decisively determined the crystal structure and Mo/Ln coordination for the two families of compounds. NH4Ln(MoO4)2 was analyzed to be orthorhombic (Pbcn space group, no. 60) and monoclinic (P2/c, no. 13) for the larger and smaller Ln3+ of Ln = La-Gd and Ln = Tb-Lu (including Y), respectively, where both the crystal structures have a layered topology featured by the alternative stacking of a [Ln(MoO4)2]- three-tier infinite anionic layer and interlayer NH4+. Four types of crystal structures were found for the Ln2Mo4O15 series, which are monoclinic (P21/a, no. 14) for Ln = La, triclinic (P1̅, no. 2) for Ln = Pr-Sm, triclinic (P1̅, no. 2) for Ln = Eu and Gd, and monoclinic (P21/c, no. 14) for Ln = Tb-Yb (including Y). The photoluminescence of NH4Ln(MoO4)2 (Ln = Eu, Tb) and Ln2Mo4O15:Eu3+ (Ln = La, Gd, Y) was thoroughly investigated in terms of spectral features, quantum efficiency, fluorescence decay, and CIE chromaticity. The thermal stability of luminescence was also studied for Ln2Mo4O15:Eu3+, and the observed charge-transfer excitation components were successfully correlated with the features of the Mo-O polyhedron/unit.

14.
Molecules ; 27(2)2022 Jan 14.
Artigo em Inglês | MEDLINE | ID: mdl-35056841

RESUMO

Constructing excited-state intermolecular proton transfer (ESIPT-e) fluorophores represents significant challenges due to the harsh requirement of bearing a proton donor-acceptor (D-A) system and their matching proton donating-accepting ability in the same molecule. Herein, we synthesized a new-type ESIPT-e fluorophor (2-APC) using the "four-component one-pot" reaction. By the installing of a cyano-group on pyridine scaffold, the proton donating ability of -NH2 was greatly enhanced, enabling 2-APC to undergo ESIPT-e process. Surprisingly, 2-APC exhibited dual-emissions in protic solvents ethanol and normal fluorescence in aprotic solvents, which is vastly different from that of conventional ESIPT-a dyes. The ESIPT emission can be obviously suppressed by Fe3+ due to the coordination reaction of Fe3+ with the A-D system in 2-APC. From this basis, a highly sensitive and selective method was established using 2-APC as a fluorescent probe, which offers the sensitive detection of Fe3+ ranging from 0 to 13 µM with the detection limit of 7.5 nM. The recovery study of spiked Fe3+ measured by the probe showed satisfactory results (97.2103.4%) with the reasonable RSD ranging from 3.1 to 3.8%. Moreover, 2-APC can also exhibit aggregation-induced effect in poor solvent or solid-state, eliciting strong red fluorescence. 2-APC was also applied to cell-imaging, exhibiting good cell-permeability, biocompatibility and color rendering. This multi-mode emission of 2-APC is significant departure from that of conventional extended p-conjugated systems and ESIPT dyes based on a flat and rigid molecular design. The "one-pot synthesis" strategy for the construction of ESIPT molecules pioneered a new route to achieve tricolor-emissive fluorophores.


Assuntos
Técnicas Biossensoriais/métodos , Corantes Fluorescentes/química , Ferro/análise , Neoplasias Pulmonares/metabolismo , Prótons , Solventes/química , Poluentes Químicos da Água/análise , Células A549 , Proliferação de Células , Transferência de Energia , Humanos , Neoplasias Pulmonares/patologia , Imagem Molecular , Espectrometria de Fluorescência/métodos
15.
Angew Chem Int Ed Engl ; 61(29): e202203358, 2022 07 18.
Artigo em Inglês | MEDLINE | ID: mdl-35363416

RESUMO

Manipulation of a multi-physical quantity to steer a molecular photophysical property is of great significance in improving sensing performance. Here, an investigation on how a physical quantity rooted in the molecular structure induces an optical behavior change to facilitate ultrasensitive detection of ethylenediamine (EDA) is performed by varying a set of thiols. The model molecule consisting of a thiol with dual-carboxyl exhibits the strongest fluorescence, which is ascribed to the electron-donating ability and prompted larger orbital overlap and oscillator strength. The elevated fluorescence positively corelated to the increased EDA, endowing an ultrasensitive response to the nanomolar-liquid/ppm-vapor. A gas detector with superior performance fulfills a contactless and real-time management of EDA. We envisage this electron-tuning strategy-enabled fluorescence enhancement can offer in-depth insight in advancing molecule-customized design, further paving the way to widening applications.


Assuntos
Corantes , Etilenodiaminas , Eletrônica , Etilenodiaminas/química , Espectrometria de Fluorescência , Compostos de Sulfidrila
16.
Inorg Chem ; 60(13): 9773-9784, 2021 Jul 05.
Artigo em Inglês | MEDLINE | ID: mdl-34134483

RESUMO

By stabilization of the Gd3Al5O12 garnet by replacing 80% or more of Al3+ with Mg2+/Ge4+ pairs, a series of new orange-yellow-emitting Gd3MgxGexAl5-2xO12:Ce (x = 2.0-2.5) phosphors were successfully developed for potential application in warm-white-light-emitting diodes (WLEDs). Rietveld structure refinement proved that Mg2+ first substitutes the octahedral Al3+ ion, followed by the replacement of the tetrahedral Al3+ together with Ge4+. The band structure of the x = 2.0 typical garnet was analyzed via density functional theory (DFT) calculations. The incorporation of an increasing content of Mg2+/Ge4+ was experimentally shown to narrow the band gap and expand the unit cell of the garnet host and blue shift the emission/excitation wavelength and shorten the fluorescence lifetime of Ce3+. The photoluminescence behaviors were rationalized by considering the influence of Mg2+/Ge4+ on the crystal structure, band structure, and local coordination. An LED lamp fabricated by combining the (Gd2.97Ce0.03)Mg2Ge2AlO12 optimal phosphor with a 450 nm-emitting InGaN blue LED chip exhibited a color-rendering index of 71.6, luminous efficacy of 16.1 lm/W, and a low correlated color temperature of 2201 K under a driving current of 20 mA, indicating that phosphor may have potential application in warm WLEDs.

17.
J Ultrasound Med ; 40(11): 2441-2448, 2021 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-33433027

RESUMO

OBJECTIVES: To evaluate shear wave elastography (SWE) technology diagnosis value of endometrial cancer (EC) and atypical endometrial hyperplasia (AEH), and to establish predictive logistic regression models for the diagnosis of EC and AEH. METHODS: Clinical information collection, transvaginal conventional ultrasonography, and SWE check were performed on 122 patients, who were perimenopausal or postmenopausal vaginal bleeding with ≥4.5 mm thick endometrium. The maximal (Emax) and mean (Emean) of Young's modulus for the endometrium were obtained. Using pathology as the gold standard, ROC curves were plotted to evaluate Young's modulus on the diagnostic effectiveness of EC and AEH. Single-factor analysis and bivariate logistic regression methods were applied to assess the clinical variables, transuaginal conventional ultrasonography variables, and Young's modulus on the identification of EC and AEH. RESULTS: Out of 122 cases of endometrial lesions, 85 cases were benign lesions, and the remaining 37 cases were EC and AEH. The Emax and Emean for the benign group were 29.80 ± 11.40 and 17.96 ± 8.05 kPa, respectively. The Emax and Emean values for EC and AEH group were 59.49 ± 16.95 and 38.46 ± 17.10 kPa, respectively. Emax and Emean for both groups were statistically significant, with p <.001. In the logistical regression analysis, endometrial thickness, Color score, and Young's modulus were identified as independent risk factors for EC and AEH. CONCLUSIONS: SWE technology plays an important role in the diagnosis of EC and AEH, and the diagnostic effectiveness would be higher when combined with conventional ultrasonography.


Assuntos
Técnicas de Imagem por Elasticidade , Hiperplasia Endometrial , Neoplasias do Endométrio , Módulo de Elasticidade , Hiperplasia Endometrial/diagnóstico por imagem , Neoplasias do Endométrio/diagnóstico por imagem , Feminino , Humanos , Fatores de Risco
18.
Anal Chem ; 92(20): 13980-13988, 2020 10 20.
Artigo em Inglês | MEDLINE | ID: mdl-32938181

RESUMO

Although colorimetric detection based on reagents has been widely used in the fields of practical trace analysis, its versatility for detecting multitargets remains the most challenging problem. As a proof of concept, a general colorimetric reagent based on potassium isopropanol (C3H7KO) and dimethyl sulfoxide for one-step instantaneous detection and discrimination of typical military and improvised explosives was designed. Vivid colors from none to purple red, blue green, yellow green, and green were shown, respectively, when detecting 2,4,6-trinitrotoluene (TNT), 2,4-dinitrotoluene (DNT), elemental sulfur (S), and potassium permanganate (KMnO4). The unique design including the specific nucleophilic addition reaction and the base-catalyzed oxidation-induced electron transfer ensures perfect selectivity even upon facing more than 20 interferents. It is further experimentally demonstrated that the confinement effect introduced by Tween-20 plays an essential role in enhancing the color signal on the surface and thus boosts the detection performance even with a mass as low as 1.45 ng. The applicability of this versatile colorimetric reagent was further verified by integrating the reagent onto paper strips for the in-field identification of TNT, DNT, S, and KMnO4 with the help of a portable smartphone-based microscope apparatus, and a practical detection mass of 10.3 ng could be realized. We expect the present colorimetric reagent design strategy would pave a way for one-step instantaneous visual detection toward trace multianalytes.


Assuntos
Colorimetria/métodos , Substâncias Explosivas/análise , Cor , Dinitrobenzenos/análise , Limite de Detecção , Polissorbatos/química , Permanganato de Potássio/análise , Trinitrotolueno/análise
19.
Mikrochim Acta ; 187(11): 617, 2020 10 19.
Artigo em Inglês | MEDLINE | ID: mdl-33074405

RESUMO

A novel magnetic hollow bimetallic zinc/cobalt-based zeolitic imidazolate framework (MHB-Zn/Co-ZIF-8) was prepared via a microwave-assisted chemical etching in methanol. The structure, morphology, and specific surface area were characterized by X-ray diffraction and FTIR spectroscopy, scanning and transmission electron microscopy, and N2 adsorption. The hollow nanostructures with high internal specific surface area, abundant active sites, and reduced aggregation of nanoparticles endow the hollow zeolitic imidazolate framework (ZIF) nanoparticle with high chemical stability, desirable durability, and excellent adsorption abilities. The MHB-Zn/Co-ZIF-8 nanoparticle was used as an effective sorbent for magnetic solid-phase extraction (MSPE) of trace aflatoxins B1, B2, G1, and G2 from fruit juice and fruit samples. The main parameters affecting the efficiency of MSPE procedures were investigated and optimized. The results show that, under optimized conditions, enrichment factors ranging from 67- to 355-fold are obtained for the target analytes. The method is linear in the range 1.0 to 100.0 ng mL-1 with correlation coefficients (R2) from 0.9960 to 0.9992. The limits of detection of four aflatoxins are in the range 0.18 to 1.50 ng mL-1 and the average recoveries range from 75.1 to 102.4%, with relative standard deviations (RSDs) less than 13.6%. This work presents the excellent extraction performance of aflatoxins B1, B2, G1, and G2 on MHB-Zn/Co-ZIF-8. In addition, the applicability of the MSPE coupling with ultrahigh-performance liquid chromatography-ion trap tandem mass spectrometry (UHPLC-IT-MSn) for trace analysis in complex matrices is shown. Graphical abstract Schematic presentation of magnetic hollow bimetallic zinc/cobalt zeolitic imidazolate framework as sorbent for efficiently enriching aflatoxins B1, B2, G1, and G2 from fruit juice samples prior to ultrahigh-performance liquid chromatography-ion trap tandem mass spectrometry (UHPLC-IT-MSn) determination.

20.
Inorg Chem ; 58(14): 9432-9442, 2019 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-31241327

RESUMO

Tartrate (Tar2-) was originally employed in this work as a chelating/structure-directing agent for hydrothermal crystallization of ZnWO4, where the decisive roles of Tar2-/Zn2+/WO42- molar ratio, solution pH (7-10), and the use of ethylene glycol (EG) cosolvent in phase/morphology evolution were deciphered in detail. It was unambiguously manifested that Tar2- may remarkably retard the intrinsically preferred [001] growth of ZnWO4, transform 1D nanorods to 0D nanoparticles and then to 2D platelets, and meanwhile induce face-to-face alignment of the platelets to form spheroidal, ellipsoidal and snowflakelike 3D architectures, where the 2D crystallites were revealed to develop via oriented attachment (colattice) of non-(00l) facets. A lower solution pH and excessive WO42- were clearly shown to enhance and offset the effect of Tar2-, which led to ellipsoidal assemblies of substantially larger 2D crystallites and suppressed 2D growth/3D assembly of ZnWO4 crystallites, respectively. With the spheroidal architectures for example, doping ZnWO4 with RE3+ yielded (Zn0.98RE0.02)WO4 phosphors (RE = Sm, Eu, Tb, and Dy, respectively) that show luminescence overlapped from the typical linelike and broad-band (∼350-700 nm) emissions of RE3+ and WO6, respectively. The luminescence color of the sample was found to drift away from the blue corner of the CIE chromaticity diagram with RE3+ doping and to be dependent on the type of RE3+.

SELEÇÃO DE REFERÊNCIAS
Detalhe da pesquisa