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1.
Front Chem ; 12: 1427451, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38952891

RESUMO

In solid propellants, combustion catalysts play a crucial role. Here, we introduce a convenient method for the self-assembly of UIO-66 (Mn) in the presence of water, leading to the preparation of Mn/C aerogels. The aerogels were successfully utilized in the thermocatalytic decomposition of ammonium perchlorate (AP). The results indicate that the incorporation of 2% mass fraction of Mn/C aerogels enhances the peak temperature of AP decomposition by approximately 87.5°C. Mn/C aerogels demonstrate excellent catalytic performance. In combination with kinetics, we propose a thermal catalytic mechanism.

2.
Artigo em Inglês | MEDLINE | ID: mdl-38991175

RESUMO

Enrichment and quantification of sugar phosphates (SPx) in biological samples were of great significance in biological medicine. In this work, a series of zirconium-based metal-organic frameworks (MOFs) with different degrees of defects, namely, HP-UiO-66-NH2-X, were synthesized using acetic acid as a modulator and were utilized as high-capacity adsorbents for the adsorption of SPx in biological samples. The results indicated that the addition of acetic acid altered the morphology of HP-UiO-66-NH2-X, with corresponding changes in pore size (3.99-9.28 nm) and specific surface area (894.44-1142.50 m2·g-1). HP-UiO-66-NH2-10 showed the outstanding performance by achieving complete adsorption of all four SPx using only 80 µg of the adsorbent. The excellent adsorption efficiency of HP-UiO-66-NH2-10 was also obtained with a wide pH range and short adsorption time (10 min). Adsorption experiments demonstrated that the adsorption process involved chemical adsorption and multilayer adsorption. By utilizing X-ray photoelectron spectroscopy and density functional theory to explain the adsorption mechanism, it was found that various interactions (including coordination, hydrogen bonding, and electrostatic interactions) collectively contributed to the exceptional adsorption capability of HP-UiO-66-NH2-10. Those results indicated that the defect strategy not only increased the specific surface area and pore size, providing additional adsorption sites, but also reduced the adsorption energy between HP-UiO-66-NH2-10 and SPx. Moreover, HP-UiO-66-NH2-10 showed a low limit of detection (0.001-0.01 ng·mL-1), high precision (<13.77%), and accuracy (80.10-111.83%) in serum, liver, and cells, good stability, high selectivity (SPx/glucose, 1:100 molar ratio), and high adsorption capacity (292 mg·g-1 for SPx). The practical detection of SPx from human serum was also verified, prefiguring the great potentials of defective zirconium-based MOFs for the enrichment and detection of SPx in the biological medicine.

3.
Adv Sci (Weinh) ; : e2404931, 2024 Jul 08.
Artigo em Inglês | MEDLINE | ID: mdl-38976515

RESUMO

The intensive study of electrochemical CO2 reduction reaction (CO2RR) has resulted in numerous highly selective catalysts, however, most of these still exhibit uncontrollable selectivity. Here, it is reported for the first time the controllable CH4/C2H4 selectivity by modulating the electronic states of Cu incorporated in metal-organic frameworks with different functional ligands, achieving a Faradaic efficiency of 58% for CH4 on Cu-incorporated UiO-66-H (Ce) composite catalysts, Cu/UiO-66-H (Ce) and that of 44% for C2H4 on Cu/UiO-66-F (Ce). In situ measurements of Raman and X-ray absorption spectra revealed that the electron-withdrawing ability of the ligand side group controls the product selectivity on MOFs through the modulation of the electronic states of Cu. This work opens new prospects for the development of MOFs as a platform for the tailored tuning of selectivity in CO2RR.

4.
Artigo em Inglês | MEDLINE | ID: mdl-38975983

RESUMO

Oral infectious diseases have a significant impact on the health of oral and maxillofacial regions, as well as the overall well-being of individuals. Carvacrol and thymol, two isomers known for their effective antibacterial and anti-inflammatory properties, have gained considerable attention in the treatment of oral infectious diseases. However, their application as topical drugs for oral use is limited due to their poor physical and chemical stability. UiO-66, a metal-organic framework based on zirconium ion (Zr4+), exhibits high drug loading capability. Carvacrol and thymol were efficiently loaded onto UiO-66 with loading rates of 79.60 ± 0.71% and 79.65 ± 0.76%, respectively. The release rates of carvacrol and thymol were 77.82 ± 0.87% and 76.51 ± 0.58%, respectively, after a period of 72 h. Moreover, Car@UiO-66 and Thy@UiO-66 demonstrated excellent antibacterial properties against Candida albicans, Escherichia coli, and Staphylococcus aureus with minimum bactericidal concentrations (MBC) of 0.313 mg/mL, 0.313 mg/mL, and 1.25 mg/mL, respectively. Furthermore, based on the results of the CCK8 cytotoxicity assay, even at concentrations as high as 1.25 mg/mL, Car@UiO-66 and Thy@UiO-66 exhibited excellent biocompatibility with a relative cell survival rate above 50%. These findings suggest that Car@UiO-66 and Thy@UiO-66 possess favorable biocompatibility properties without significant toxicity towards periodontal membrane cells. Additionally, in vivo studies confirmed the efficacy of Car@UiO-66and Thy@UiO-66 in reducing inflammation, promoting bone formation through inhibition of TNF-a and IL6 expression, enhancement of IL10 expression, and acceleration of bone defect healing. Therefore, the unique combination of antibacterial, anti-inflammatory, and osteogenic properties make Car@UiO-66 and Thy@Ui O-66 promising candidates for the treatment of oral infectious diseases and repairing bone defects.

5.
ACS Appl Mater Interfaces ; 16(26): 34020-34029, 2024 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-38961571

RESUMO

Rechargeable aqueous Zn-ion batteries with a Zn anode hold great promise as promising candidates for advanced energy storage systems. The construction of protective layer coatings on Zn anode is an effective way to suppress the growth of Zn dendrites and water-induced side reactions. Herein, we reported a series of UIO-66 materials with different concentrations of reduced graphene oxide (rG) coated onto the surface of Zn foil (Zn@UIO-66/rGx; x = 0.05, 0.1, and 0.2). Benefiting from the synergistic effect of UIO-66 and rG, symmetric cells with Zn@UIO-66/rGx (x = 0.1) electrodes exhibit excellent reversibility (e.g., long cycling life over 1100 h at 1 mA cm-2/1 mAh cm-2) and superior rate capability (e.g., over 1100 and 400 h at 5 mA cm-2/2.5 mAh cm-2 and 10 mA cm-2/5 mAh cm-2, respectively). When the Zn@UIO-66/rG0.1 anode was paired with the NaV3O8·1.5H2O (NVO) cathode, the Zn@UIO-66/rG0.1||NVO cell also delivered a high reversible capacity of 189.9 mAh g-1 with an initial capacity retention of 61.3% after 500 cycles at 1 A g-1, compared to the bare Zn||NVO cell with only 92 cycles.

6.
Small ; : e2402819, 2024 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-38837885

RESUMO

Janus-micromotors, as efficient self-propelled materials, have garnered considerable attention for their potential applications in non-agitated liquids. However, the design of micromotors is still challenging and with limited approaches, especially concerning speed and mobility in complex environments. Herein, a two-step spray-drying approach encompassing symmetrical assembly and asymmetrical assembly is introduced to fabricate the metal-organic framework (MOF) Janus-micromotors with hierarchical pores. Using a spray-dryer, a symmetrical assembly is first employed to prepare macro-meso-microporous UiO-66 with intrinsic micropores (<0.5 nm) alongside mesopores (≈24 nm) and macropores (≈400 nm). Subsequent asymmetrical assembly yielded the UiO-66-Janus loaded with the reducible nanoparticles, which underwent oxidation by KMnO4 to form MnO2 micromotors. The micromotors efficiently generated O2 for self-propulsion in H2O2, exhibiting ultrahigh speeds (1135 µm s-1, in a 5% H2O2 solution) and unique anti-gravity diffusion effects. In a specially designed simulated sand-water system, the micromotors traversed from the lower water to the upper water through the sand layer. In particular, the as-prepared micromotors demonstrated optimal efficiency in pollutant removal, with an adsorption kinetic coefficient exceeding five times that of the micromotors only possessing micropores and mesopores. This novel strategy fabricating Janus-micromotors shows great potential for efficient treatment in complex environments.

7.
Int J Mol Sci ; 25(12)2024 Jun 20.
Artigo em Inglês | MEDLINE | ID: mdl-38928488

RESUMO

The oxidative esterification of aldehydes under mild conditions remains a significant challenge. This study introduces a unique defective UiO-66 to achieve gold nanoclusters (AuNCs) for efficient aldehyde oxidation under mild conditions. The construction and characterization of these materials are thoroughly investigated by techniques of XRD, SEM and TEM images, FT-IR, Raman, and XPS spectrum, emphasizing the unique microporous in defective UiO-66 are conducive to the fabrication of AuNCs. The catalytic performance of the prepared materials in aldehyde oxidation reactions is systematically evaluated, demonstrating the remarkable efficiency of dispersed Au@UiO-66-25 with high-content (9.09 wt%) Au-loading and ultra-small size (~2.7 nm). Moreover, mechanistic insights into the catalytic process under mild conditions (70 °C for 1 h) are provided, elucidating the determination of defective UiO-66 in the confined fabrication of AuNCs and subsequent furfural adsorption, which underlie the principles governing the observed enhancements. This study establishes the groundwork for the synthesis of highly dispersed and catalytically active metal nanoparticles using defective MOFs as a platform, advancing the catalytic esterification reaction of furfural to the next level.


Assuntos
Aldeídos , Ouro , Nanopartículas Metálicas , Oxirredução , Ouro/química , Nanopartículas Metálicas/química , Aldeídos/química , Catálise , Estruturas Metalorgânicas/química , Porosidade , Esterificação , Espectroscopia de Infravermelho com Transformada de Fourier
8.
Molecules ; 29(11)2024 May 25.
Artigo em Inglês | MEDLINE | ID: mdl-38893383

RESUMO

The thermally stable zirconium-based MOF, UiO-66, was employed for the preparation of bonded porous-layer open-tubular (PLOT) GC columns. The synthesis included the in situ growth of the UiO-66 film on the inner wall of the capillary through a one-step solvothermal procedure. SEM-EDX analysis revealed the formation of a thin, continuous, uniform, and compact layer of UiO-66 polycrystals on the functionalized inner wall of the column. The average polarity (ΔIav = 700) and the McReynolds constants reflected the polar nature of the UiO-66 stationary phase. Several mixtures of small organic compounds and real samples were used to evaluate the separation performance of the fabricated columns. Linear alkanes from n-pentane to n-decane were baseline separated within 1.35 min. Also, a series of six n-alkylbenzenes (C3-C8) were separated within 3 min with a minimum resolution of 3.09, whereas monohalobenzene mixtures were separated at 220 °C within 14s. UiO-66 PLOT columns are ideally suited for the isothermal separation of chlorobenzene structural isomers at 210 °C within 45 s with Rs ≥ 1.37. The prepared column featured outstanding thermal stability (up to 450 °C) without any observed bleeding or significant impact on its performance. This feature enabled the analysis of various petroleum-based samples.

9.
Talanta ; 277: 126400, 2024 Jun 10.
Artigo em Inglês | MEDLINE | ID: mdl-38876031

RESUMO

Captopril (CP) is commonly used as an active enzyme inhibitor for the treatment of coronary heart disease, hypertension and angina pectoris. The development of sensitive and efficient method for CP analysis is of great importance in biomedical research. Herein, we fabricated a sensitive and robust hydrogel-assisted paper-based sensor based on fluorescence UiO-66-NH2@ZIF-8 and Co, N-doped carbon nanozymes with oxidase-mimicking activity for accurate monitoring of captopril. The hydrogel-assisted paper-based sensor appeared a visible pink signal due to the catalytic oxidation of colorless N,N-diethyl-p-phenylenediamine (DPD) to oxDPD by Co, N-doped carbon-based nanozymes, and resulted in the fluorescence quenching of UiO-66-NH2@ZIF-8. In the presence of captopril, the oxidation of chromogenic substrate DPD by Co, N-doped nanozymes in the hydrogel-assisted paper-based sensor was hindered and accompanied by a change in the visible color, leading to recovery of the fluorescence of UiO-66-NH2@ZIF-8, and the change in the fluorescence color could also be observed. Therefore, the quantitative detection of captopril is achieved by taking a smartphone photograph and converting the image parameters into data information using ImageJ software. The portable hydrogel-assisted paper sensor provided sensitive detection of captopril in two modes based on visible color change as well as fluorescence color change with limits of detection of 0.45 µM and 0.47 µM, respectively. This hydrogel-assisted paper-based sensor has been successfully applied to the accurate monitoring of captopril in human serum, providing a potential avenue for in situ detection of captopril.

10.
Int J Biol Macromol ; 269(Pt 1): 131988, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38701999

RESUMO

The disposal of waste lithium batteries, especially waste separators, has always been a problem, incineration and burial will cause environmental pollution, therefore, the development of degradable and high-performance separators has become an important challenge. Herein, UiO-66-NH2 particles were successfully anchored onto bacterial cellulose (BC) separators by epichlorohydrin (ECH) as a crosslinker, then a BC/UiO-66-NH2 composite separator was prepared by vacuum filtration. The ammonia groups (-NH2) from UiO-66-NH2 can form hydrogen bonds with PF6- in the electrolyte, promoting lithium-ion transference. Additionally, UiO-66-NH2 can store the electrolyte and tune the porosity of the separator. The lithium ion migration number (0.62) of the battery assembled with BC/UiO-66-NH2 composite separator increased by 50 % compared to the battery assembled with commercial PP separator (0.45). The discharge specific capacity of the battery assembled with BC/UIO-66-NH2 composite separator after 50 charge and discharge cycles is 145.4 mAh/g, which is higher than the average discharge specific capacity of 114.3 mAh/g of the battery assembled with PP separator. When the current density is 2C, the minimum discharge capacity of the battery assembled with BC/UiO-66-NH2 composite separator is 85.3 mAh/g. The electrochemical performance of the BC/UiO-66-NH2 composite separator is significantly better than that of the commercial PP separator. In addition, -NH2 can offer a nitrogen source to facilitate degradation of the BC separators, whereby the BC/UiO-66-NH2 composite separator could be completely degraded in 15 days.


Assuntos
Celulose , Fontes de Energia Elétrica , Lítio , Lítio/química , Celulose/química , Íons/química , Biodegradação Ambiental
11.
ACS Appl Mater Interfaces ; 16(20): 26685-26712, 2024 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-38722359

RESUMO

The ubiquitous presence of pharmaceutical pollutants in the environment significantly threatens human health and aquatic ecosystems. Conventional wastewater treatment processes often fall short of effectively removing these emerging contaminants. Therefore, the development of high-performance adsorbents is crucial for environmental remediation. This research utilizes molecular simulation to explore the potential of novel modified metal-organic frameworks (MOFs) in pharmaceutical pollutant removal, paving the way for the design of efficient wastewater treatment strategies. Utilizing UIO-66, a robust MOF, as the base material, we developed UIO-66 functionalized with chitosan (CHI) and oxidized chitosan (OCHI). These modified MOFs' physical and chemical properties were first investigated through various characterization techniques. Subsequently, molecular dynamics simulation (MDS) and Monte Carlo simulation (MCS) were employed to elucidate the adsorption mechanisms of rosuvastatin (ROSU) and simvastatin (SIMV), two prevalent pharmaceutical pollutants, onto these nanostructures. MCS calculations demonstrated a significant enhancement in the adsorption energy by incorporating CHI and OCHI into UIO-66. This increased ROSU from -14,522 to -16,459 kcal/mol and SIMV from -17,652 to -21,207 kcal/mol. Moreover, MDS reveals ROSU rejection rates in neat UIO-66 to be at 40%, rising to 60 and 70% with CHI and OCHI. Accumulation rates increase from 4 Å in UIO-66 to 6 and 9 Å in UIO-CHI and UIO-OCHI. Concentration analysis shows SIMV rejection surges from 50 to 90%, with accumulation rates increasing from 6 to 11 Å with CHI and OCHI in UIO-66. Functionalizing UIO-66 with CHI and OCHI significantly enhanced the adsorption capacity and selectivity for ROSU and SIMV. Abundant hydroxyl and amino groups facilitated strong interactions, improving performance over that of unmodified UIO-66. Surface functionalization plays a vital role in customizing the MOFs for pharmaceutical pollutant removal. These insights guide next-gen adsorbent development, offering high efficiency and selectivity for wastewater treatment.


Assuntos
Quitosana , Estruturas Metalorgânicas , Simulação de Dinâmica Molecular , Nanoestruturas , Rosuvastatina Cálcica , Sinvastatina , Poluentes Químicos da Água , Quitosana/química , Estruturas Metalorgânicas/química , Sinvastatina/química , Rosuvastatina Cálcica/química , Adsorção , Poluentes Químicos da Água/química , Poluentes Químicos da Água/isolamento & purificação , Nanoestruturas/química , Oxirredução , Ácidos Ftálicos
12.
Sci Total Environ ; 932: 172941, 2024 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-38703844

RESUMO

Different Br-doped metal-organic frameworks (MOFs) derived (Brx@UiO-66) have been prepared by heat treatment using UiO-66 as the precursor. The experimental results showed that Br0.2@UiO-66 exhibited the best photocatalytic oxidation and adsorption performances toward acetaldehyde. In the dynamic system, the acetaldehyde removal rate and adsorption capacity of Br0.2@UiO-66 were 93.2 % and 230.59 mg/g, respectively. The improvement of the photocatalytic performance can be attributed to the presence of Br ions and CBr bonds, which facilitated the rapid separation of electrons and holes and the production of •O2-. In addition, Br0.2@UiO-66 had a better adsorption performance than 300UiO-66, mainly because of the increased Lewis acidity of the metal active sites due to Br doping. Radical capture experiments indicated that •O2- and e- were the primary active substances in acetaldehyde oxidation, and allowed establishing the possible mechanism of acetaldehyde oxidation. This work shows that MOFs can have high catalytic oxidation performances toward volatile organic compounds (VOCs) while retaining their adsorption capacity, and can be used for practical applications in the adsorption-catalytic integrated degradation of VOCs.

13.
Biosensors (Basel) ; 14(5)2024 May 04.
Artigo em Inglês | MEDLINE | ID: mdl-38785703

RESUMO

In this work, UiO-66-NH2/GO nanocomposite was prepared using a simple solvothermal technique, and its structure and morphology were characterized using field emission scanning electron microscopy (FE-SEM), energy-dispersive X-ray spectroscopy (EDS), and X-ray diffraction (XRD). An enhanced electrochemical sensor for the detection of epirubicin (EP) was proposed, which utilized a UiO-66-NH2/GO nanocomposite-modified screen-printed graphite electrode (UiO-66-NH2/GO/SPGE). The prepared UiO-66-NH2/GO nanocomposite improved the electrochemical performance of the SPGE towards the redox reaction of EP. Under optimized experimental conditions, this sensor demonstrates a remarkable limit of detection (LOD) of 0.003 µM and a linear dynamic range from 0.008 to 200.0 µM, providing a highly capable platform for sensing EP. Furthermore, the simultaneous electro-catalytic oxidation of EP and topotecan (TP) was investigated at the UiO-66-NH2/GO/SPGE surface utilizing differential pulse voltammetry (DPV). DPV measurements revealed the presence of two distinct oxidation peaks of EP and TP, with a peak potential separation of 200 mV. Finally, the UiO-66-NH2/GO/SPGE sensor was successfully utilized for the quantitative analysis of EP and TP in pharmaceutical injection, yielding highly satisfactory results.


Assuntos
Antineoplásicos , Técnicas Eletroquímicas , Eletrodos , Epirubicina , Grafite , Nanocompostos , Topotecan , Epirubicina/análise , Topotecan/análise , Grafite/química , Antineoplásicos/análise , Técnicas Biossensoriais , Estruturas Metalorgânicas/química , Limite de Detecção , Humanos , Oxirredução , Ácidos Ftálicos
14.
Mikrochim Acta ; 191(6): 304, 2024 05 06.
Artigo em Inglês | MEDLINE | ID: mdl-38710810

RESUMO

Dual-emissive fluorescence probes were designed by integrating porphyrin into the frameworks of UiO-66 for ratiometric fluorescence sensing of amoxicillin (AMX). Porphyrin integrated UiO-66 showed dual emission in the blue and red region. AMX resulted in the quenching of blue fluorescence component, attributable to the charge neutralization and hydrogen bonds induced energy transfer. AMX was detected using (F438/F654) as output signals. Two linear relationships were observed (from 10 to 1000 nM and 1 to 100 µM), with a limit of detection of 27 nM. The porphyrin integrated UiO-66 probe was used to detect AMX in practical samples. This work widens the road for the development of dual/multiple emissive fluorescence sensors for analytical applications, providing materials and theoretical supporting for food, environmental, and human safety.


Assuntos
Amoxicilina , Antibacterianos , Corantes Fluorescentes , Leite , Porfirinas , Espectrometria de Fluorescência , Leite/química , Porfirinas/química , Antibacterianos/análise , Antibacterianos/química , Amoxicilina/análise , Amoxicilina/química , Corantes Fluorescentes/química , Animais , Espectrometria de Fluorescência/métodos , Limite de Detecção , Estruturas Metalorgânicas/química , Resíduos de Drogas/análise , Contaminação de Alimentos/análise
15.
Chempluschem ; : e202400107, 2024 May 06.
Artigo em Inglês | MEDLINE | ID: mdl-38708570

RESUMO

Metal-organic frameworks (MOF) hold great promise for CO2 adsorption due to their high surface areas, tunable pore sizes, and the ability to modify their chemical properties to enhance CO2 affinity. MOFs tagged with functional groups either at linker or metal sites have shown improved CO2 uptake capacity and selectivity. This study focuses on investigating the potential of selective CO2 adsorption using amino functionalization of linker forming Ce-UiO-66. The physicochemical properties and characteristics of MOFs to determine the degree of amino functionalization and structural stability were examined using powder X-ray diffraction (PXRD), Fourier transformer infra-red (FTIR), scanning electron microscopy (SEM), thermogravimetric analysis (TGA), and N2 porosimetry and specific surface area (BET). This work unveils a novel array of results on CO2, N2 and water vapour adsorption on Ce-UiO-66-NH2. The amino-functionalized Ce-UiO-66-NH2 shows 63 % higher CO2 uptake and 84 % higher CO2/N2 selectivity at 273 K and 1 bar over Ce-UiO-66. Ce-UiO-66-NH2 also shows excellent structural stability after gas and vapour sorption making Ce-UiO-66-NH2 potential adsorbent for CO2 capture.

16.
Talanta ; 274: 125999, 2024 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-38583327

RESUMO

The construction of efficient methods for highly sensitive and rapid detection of disease markers is essential for the early diagnosis of serious diseases. In this paper, taking advantage of the UiO-66-NH2 signal molecule in combination with a waste-free entropy-driven DNA machine, a novel homogeneous electrochemical ratiometric platform is developed to detect MircoRNA (miRNA). Metal-organic framework materials (UiO-66-NH2 MOF) and ferrocene were utilized as electrochemical signal tags and reference probes, respectively. The target-initiated waste-free three-dimensional (3D) entropy-driven DNA nanomachine is activated in the presence of miRNA, resulting in DNA-labeled-UiO-66-NH2 falling off from the electrode, leading to a decrease in the signal of UiO-66-NH2 at 0.83V. Our strategy can mitigate false positive responses induced by the DNA probes immobilized on electrodes in traditional distance-dependent signal adjustment ratiometric strategies. The proposed ratiometric platform demonstrates superior sensitivity (a detection limit of 9.8 fM), simplified operation, high selectivity, and high repeatability. The ratiometric biosensor is also applied to detect miRNA content in spiked serum samples.


Assuntos
Técnicas Biossensoriais , Técnicas Eletroquímicas , Entropia , Estruturas Metalorgânicas , MicroRNAs , MicroRNAs/sangue , MicroRNAs/análise , Técnicas Biossensoriais/métodos , Técnicas Eletroquímicas/métodos , Humanos , Estruturas Metalorgânicas/química , DNA/química , Limite de Detecção , Eletrodos , Sondas de DNA/química , Sondas de DNA/genética , Compostos Ferrosos/química , Metalocenos/química
17.
Talanta ; 274: 126039, 2024 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-38604043

RESUMO

The development of intelligent, sensitive, and visual methods for the rapid detection of veterinary drug residues is essential to ensure food quality and safety. Here, a smartphone-based dual inverse signal MOFs fluorescence sensing system was proposed for intelligent in-site visual detection of malachite green (MG). A UiO-66-NH2@RhB-dual-emission fluorescent probe was successfully synthesized in one step using a simple one-pot method. The inner filter effect (IFE) quenches the red fluorescence, while hydrogen bonding interaction enhances the blue fluorescence, enabling highly sensitive, accurate, and visual detection of MG dual inverse signals through fluorescence analysis. The probe showed great linearity over a wide range of 0.1-100 µmol/L, with a limit of detection (LOD) of 20 nmol/L. By integrating smartphone photography and RGB (red, green, and blue) analysis, accurate quantitative analysis of MG in water and actual fish samples can be achieved within 5 min. This developed platform holds great promise for the on-site detection of MG in practical applications, with the advantages of simplicity, cost-effectiveness, and rapidity. Consequently, it may open up a new pathway for on-site evaluation of food safety and environmental health.


Assuntos
Corantes Fluorescentes , Corantes de Rosanilina , Smartphone , Corantes de Rosanilina/análise , Corantes de Rosanilina/química , Corantes Fluorescentes/química , Espectrometria de Fluorescência/métodos , Animais , Limite de Detecção , Fluorescência , Peixes , Poluentes Químicos da Água/análise
18.
Artigo em Inglês | MEDLINE | ID: mdl-38669483

RESUMO

The need to develop green and cost-effective industrial catalytic processes has led to growing interest in preparing more robust, efficient, and selective heterogeneous catalysts at a large scale. In this regard, microwave-assisted synthesis is a fast method for fabricating heterogeneous catalysts (including metal oxides, zeolites, metal-organic frameworks, and supported metal nanoparticles) with enhanced catalytic properties, enabling synthesis scale-up. Herein, the synthesis of nanosized UiO-66-NH2 was optimized via a microwave-assisted hydrothermal method to obtain defective matrices essential for the stabilization of metal nanoparticles, promoting catalytically active sites for hydrogenation reactions (760 kg·m-3·day-1 space time yield, STY). Then, this protocol was scaled up in a multimodal microwave reactor, reaching 86% yield (ca. 1 g, 1450 kg·m-3·day-1 STY) in only 30 min. Afterward, Pd nanoparticles were formed in situ decorating the nanoMOF by an effective and fast microwave-assisted hydrothermal method, resulting in the formation of Pd@UiO-66-NH2 composites. Both the localization and oxidation states of Pd nanoparticles (NPs) in the MOF were achieved using high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray photoelectron spectroscopy (XPS), respectively. The optimal composite, loaded with 1.7 wt % Pd, exhibited an extraordinary catalytic activity (>95% yield, 100% selectivity) under mild conditions (1 bar H2, 25 °C, 1 h reaction time), not only in the selective hydrogenation of a variety of single alkenes (1-hexene, 1-octene, 1-tridecene, cyclohexene, and tetraphenyl ethylene) but also in the conversion of a complex mixture of alkenes (i.e., 1-hexene, 1-tridecene, and anethole). The results showed a powerful interaction and synergy between the active phase (Pd NPs) and the catalytic porous scaffold (UiO-66-NH2), which are essential for the selectivity and recyclability.

19.
Environ Pollut ; 351: 124026, 2024 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-38663509

RESUMO

To develop a highly efficient adsorbent to remediate and remove hexavalent chromium ions (Cr(VI)) from polluted water, cellulose acetate (CA) and chitosan (CS), along with metal oxides (titanium dioxide (TiO2) and ferroferric oxide (Fe3O4)), and a zirconium-based metal-organic framework (UiO-66) were used to fabricate the composite porous nanofiber membranes through electrospinning. The adsorption performance, influencing factors, adsorption kinetics and isotherms of composite nanofiber membranes were comprehensively investigated. The multi-layer membrane with interpenetrating nanofibers and surface functional groups enhanced the natural physical adsorption and provided potential chemical sites. The thermal stability was improved by introducing TiO2 and UiO-66. CA/CS/UiO-66 exhibited the highest adsorption capacity (118.81 mg g-1) and removal rate (60.76%), which were twice higher than those of the control. The correlation coefficients (R2) of all the composite nanofibers regressed by the Langmuir model were significantly higher than those by the Freundlich model. The pseudo-first-order kinetic curve of CA/CS composite nanofibers showed the highest R2 (0.973), demonstrating that the whole adsorption process involved a combination of strong physical adsorption and weak chemical adsorption by the amino groups of CS. However, the R2 values of the pseudo-second-order kinetic model increased after incorporating TiO2, Fe3O4, and UiO-66 into the CA/CS composite nanofiber membranes since an enhanced chemical reaction with Cr (VI) occured during the adsorption.


Assuntos
Cromo , Estruturas Metalorgânicas , Nanofibras , Titânio , Poluentes Químicos da Água , Cromo/química , Nanofibras/química , Estruturas Metalorgânicas/química , Adsorção , Poluentes Químicos da Água/química , Titânio/química , Porosidade , Biomassa , Cinética , Zircônio/química , Quitosana/química , Celulose/química , Celulose/análogos & derivados
20.
Spectrochim Acta A Mol Biomol Spectrosc ; 316: 124336, 2024 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-38678838

RESUMO

For addressing the challenges of strong affinity SERS substrate to organophosphorus pesticides (OPs), herein, a rapid water-assisted layer-by-layer heteronuclear growth method was investigated to grow uniform UiO-66 shell with controllable thickness outside the magnetic core and provide abundant defect sites for OPs adsorption. By further assembling the tailored Au@Ag, a highly sensitive SERS substrate Fe3O4-COOH@UiO-66/Au@Ag (FCUAA) was synthesized with a SERS enhancement factor of 2.11 × 107. The substrate's suitability for the actual vegetable samples (cowpeas and peppers) was confirmed under both destructive and non-destructive detection conditions, showing a strong SERS response to fenthion and triazophos, with limits of detection of 1.21 × 10-5 and 2.96 × 10-3 mg/kg in the vegetables under destructive conditions, and 0.13 and 1.39 ng/cm2 for non-destructive detection, respectively. The FCUAA substrate had high SERS performance, effective adsorption capability for OPs, and demonstrated good applicability, thus exhibiting great potential for rapid detection of trace OPs residues in the food industry.


Assuntos
Resíduos de Praguicidas , Análise Espectral Raman , Análise Espectral Raman/métodos , Resíduos de Praguicidas/análise , Verduras/química , Ouro/química , Compostos Organofosforados/análise , Compostos Organofosforados/química , Prata/química , Fention/análise , Triazóis/química , Triazóis/análise , Limite de Detecção , Organotiofosfatos/análise , Contaminação de Alimentos/análise , Adsorção
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