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1.
Environ Sci Technol ; 58(16): 7020-7031, 2024 Apr 23.
Article in English | MEDLINE | ID: mdl-38608167

ABSTRACT

Adjusting the electronic state of noble metal catalysts on a nanoscale is crucial for optimizing the performance of nanocatalysts in many important environmental catalytic reactions, particularly in volatile organic compound (VOC) combustion. This study reports a novel strategy for optimizing Pt catalysts by modifying their electronic structure to enhance the electron density of Pt. The research illustrates the optimal 0.2Pt-0.3W/Fe2O3 heterostructure with atomic-thick WO3 layers as a bulking block to electronically modify supported Pt nanoparticles. Methods such as electron microscopy, X-ray photoelectron spectroscopy, and in situ Fourier transform infrared spectroscopy confirm Pt's electron-enriched state resulting from electron transfer from atomic-thick WO3. Testing for benzene oxidation revealed enhanced low-temperature activity with moderate tungsten incorporation. Kinetic and mechanistic analyses provide insights into how the enriched electron density benefits the activation of oxygen and the adsorption of benzene on Pt sites, thereby facilitating the oxidation reaction. This pioneering work on modifying the electronic structure of supported Pt nanocatalysts establishes an innovative catalyst design approach. The electronic structure-performance-dependent relationships presented in this study assist in the rational design of efficient VOC abatement catalysts, contributing to clean energy and environmental solutions.

2.
Food Chem ; 393: 133337, 2022 Nov 01.
Article in English | MEDLINE | ID: mdl-35653990

ABSTRACT

Based on the mussel-inspired adhesive interface (Fe3O4-g-C3N4@PDA), a novel bionic metal-organic framework (Fe3O4-g-C3N4-PDA@MIL-101) was successfully prepared. The composite featured a high specific surface area and a multi-microchannel structure, as well as strong thermochemical stability. The structural property of Fe3O4-g-C3N4-PDA@MIL-101(Fe) was characterized, and the results indicated that Fe3O4, PDA, and MIL-101(Fe) were uniformly coated on the g-C3N4 surface. The adsorption and desorption of organophosphorus pesticides with Fe3O4-g-C3N4-PDA@MIL-101(Fe) were evaluated by batch experiments. This composite showed high adsorption efficiency and selective removal of coralox, phosalone, and chlorpyrifos. Under the optimal conditions, three organophosphorus pesticides were adsorbed from Chinese cabbage and green onion samples with Fe3O4-g-C3N4-PDA@MIL-101(Fe). The analytical method exhibited high sensitivity (LOD, 0.19-2.34 µg/L; LOQ, 0.65-7.82 µg/L), excellent practicality, and good stability, suggesting that Fe3O4-g-C3N4-PDA@MIL-101 was an ideal candidate magnetic adsorbent for the removal of organophosphorus pesticides in Chinese cabbage and green onion samples.


Subject(s)
Brassica , Metal-Organic Frameworks , Pesticides , Water Pollutants, Chemical , Adhesives , Adsorption , China , Metal-Organic Frameworks/chemistry , Onions , Organophosphorus Compounds , Pesticides/analysis , Water Pollutants, Chemical/analysis
3.
Food Chem ; 352: 129187, 2021 Aug 01.
Article in English | MEDLINE | ID: mdl-33652196

ABSTRACT

A novel covalent organic framework material (3DGA@COFs), for use as a solid-phase dispersion sorbent, has been synthesized for extracting organophosphorus pesticides (OPs) from vegetables. The prepared 3DGA@COFs material exhibited many advantageous features, including a large specific surface area (127.95 m2/g) and high pore volume (0.0344 cm3/g), which made it an ideal sorbent for sample pretreatment. The experimental conditions affecting extraction performance (adsorbent type, adsorbent amount, reaction time, pH, ionic concentration, and eluent) were optimized systematically. The extracted analytes were detected by HPLC-MS/MS. Under optimized conditions, the proposed method exhibited a wide linear range (0.5-100 µg/L) and low limits of detection (0.01-0.14 µg/L). The recoveries (75.40%-102.13%) satisfied the requirements for a precise detection method. The proposed method was successfully used for determining malathion, triazophos, quinalphos in lettuce, tomato and cucumber samples, thus indicating the potential of using 3DGA@COFs materials for pretreating vegetable samples.


Subject(s)
Graphite/chemistry , Hydrogels/chemistry , Metal-Organic Frameworks/chemical synthesis , Organophosphorus Compounds/isolation & purification , Pesticides/isolation & purification , Solid Phase Extraction/methods , Vegetables/chemistry , Adsorption , Chemistry Techniques, Synthetic , Food Contamination/analysis , Hydrogen-Ion Concentration , Limit of Detection , Metal-Organic Frameworks/chemistry , Organophosphorus Compounds/analysis , Organophosphorus Compounds/chemistry , Pesticides/analysis , Pesticides/chemistry , Time Factors
4.
Article in English | MEDLINE | ID: mdl-33578273

ABSTRACT

Detection of low levels of triazole fungicides in agricultural product matrices is important. Although several detection methods have been developed, all have some drawbacks, such as being time-consuming, requiring complex sample pretreatment, and consuming large volumes of organic solvents. There is an urgent need for a simple and rapid detection method for triazole fungicides. In this study, the adsorbent composite material magnetic MOFs based on Fe3O4-MWCNT was synthesized by in-situ polymerization at room temperature, and was applied to extract triazole pesticides from fruits and vegetables. High-performance liquid chromatography-tandem mass spectrometry was used for quantification. Under optimized conditions, the constructed detection method showed a low detection (LOD) of 0.52-1.83 µg/L (S/N = 3) and wide linear range of 5.00-500.00 µg/L for triazole fungicides in the fruit and vegetable samples. The method recovery for spiked fungicides (10, 50, and 100 µg/L) in cabbage, spinach, orange juice, and apple juice ranged from 62.80% to 94.20%. The constructed detection method has a lower detection limit than previously reported methods and has a higher sensitivity for triazole pesticide residues in complex matrices.


Subject(s)
Fruit and Vegetable Juices/analysis , Metal-Organic Frameworks/chemistry , Pesticide Residues , Solid Phase Extraction/methods , Triazoles , Chromatography, High Pressure Liquid , Limit of Detection , Linear Models , Magnetite Nanoparticles/chemistry , Pesticide Residues/analysis , Pesticide Residues/isolation & purification , Reproducibility of Results , Tandem Mass Spectrometry , Triazoles/analysis , Triazoles/isolation & purification
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