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1.
Proc Natl Acad Sci U S A ; 121(16): e2401148121, 2024 Apr 16.
Artigo em Inglês | MEDLINE | ID: mdl-38602914

RESUMO

The oxidation of cycloalkanes is important in the combustion of transportation fuels and in atmospheric secondary organic aerosol formation. A transient carbon-centered radical intermediate (•QOOH) in the oxidation of cyclohexane is identified through its infrared fingerprint and time- and energy-resolved unimolecular dissociation dynamics to hydroxyl (OH) radical and bicyclic ether products. Although the cyclohexyl ring structure leads to three nearly degenerate •QOOH isomers (ß-, γ-, and δ-QOOH), their transition state (TS) barriers to OH products are predicted to differ considerably. Selective characterization of the ß-QOOH isomer is achieved at excitation energies associated with the lowest TS barrier, resulting in rapid unimolecular decay to OH products that are detected. A benchmarking approach is employed for the calculation of high-accuracy stationary point energies, in particular TS barriers, for cyclohexane oxidation (C6H11O2), building on higher-level reference calculations for the smaller ethane oxidation (C2H5O2) system. The isomer-specific characterization of ß-QOOH is validated by comparison of experimental OH product appearance rates with computed statistical microcanonical rates, including significant heavy-atom tunneling, at energies in the vicinity of the TS barrier. Master-equation modeling is utilized to extend the results to thermal unimolecular decay rate constants at temperatures and pressures relevant to cyclohexane combustion.

2.
Small ; : e2400970, 2024 May 27.
Artigo em Inglês | MEDLINE | ID: mdl-38801301

RESUMO

The fabrication of materials with hierarchical structures has garnered great interest, owing to the potential for significantly enhancing their functions. Herein, a strategy of coupling molecular solvation and crystal growth is presented to fabricate porous spherulites of 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane (CL-20), an important energetic material. With the addition of polyvinylpyrrolidone in the antisolvent crystallization, the metastable solvate of CL-20 is formed and grows spherulitically, and spontaneously desolvates to obtain the porous spherulite when filtration, in which the characteristic peak of the nitro group of CL-20 shifts detected by the in situ micro-confocal Raman spectroscopy. The effect of polyvinylpyrrolidone is thought to induce the solvation of CL-20, confirmed by density functional theory calculations, meanwhile acting on the (020) face of CL-20 to trigger spherulitic growth, demonstrated through infrared spectroscopy and Rietveld refinement of powder X-ray diffraction. Moreover, compared to common CL-20 crystals, porous spherulites exhibit enhanced combustion with increases of 6.24% in peak pressure, 40.21% in pressurization rate, and 9.63% in pressure duration effect, indicating the capability of hierarchical structures to boost the energy release of energetic crystals. This work demonstrates a new route via solvation-growth coupling to construct hierarchical structures for organic crystals and provides insight into the structure-property relations for material design.

3.
Small ; : e2404623, 2024 Jul 14.
Artigo em Inglês | MEDLINE | ID: mdl-39004866

RESUMO

The high-energy (H2dabco)[NH4(ClO4)3] (DAP-4) with excellent energetic performance attracts wide attention from researchers. The investigation of its interaction with the Aluminum (Al) is of great importance. However, the higher ignition threshold of DAP-4 and the dense oxide layer (Al2O3) of Al severely limit the energy release efficiency of Al/DAP-4. In this study, a new idea to is first proposed to improve and adjust the thermal decomposition and combustion performance of Al/DAP-4 by constructing a highly dispersed iron (Fe) nanoparticle interfacial layer. It acts as a gradient catalyst to promote the thermal decomposition and combustion of DAP-4 and Al, and it also act as an oxygen transport channel to promote the contact and reaction of oxidizing gases with the internal reactive Al powder. It reduces the thermal decomposition temperature of Al@Fe-3/DAP-4 from 386.30 °C (Al/DAP-4) to 349.48 °C and leads to the vigorous combustion. Theoretical calculations show that Fe nanoparticle interfacial layer can facilitate the transport of oxygen through the established oxygen transport channels, and it can also significantly improve the energetic properties of Al@Fe-3/DAP-4 composites. In conclusion, the new approach is proposed to improve the performance of metal fuel/oxidizer composites by constructing interfacial layers, which is expected to promote their practical applications.

4.
Small ; 20(24): e2308684, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38174613

RESUMO

Porous carbon has been widely focused to solve the problems of low coulombic efficiency (ICE) and low multiplication capacity of Sodium-ion batteries (SIBs) anodes. The superior energy storage properties of two-dimensional(2D) carbon nanosheets can be realized by modulating the structure, but be limited by the carbon sources, making it challenging to obtain 2D structures with large surface area. In this work, a new method for forming carbon materials with high N/S doping content based on combustion activation using the dual activation effect of K2SO4/KNO3 is proposed. The synthesized carbon material as an anode for SIBs has a high reversible capacity of 344.44 mAh g-1 at 0.05 A g-1. Even at the current density of 5 Ag-1, the capacity remained at 143.08 mAh g-1. And the ICE of sodium-ion in ether electrolytes is ≈2.5 times higher than that in ester electrolytes. The sodium storage mechanism of ether/ester-based electrolytes is further explored through ex-situ characterizations. The disparity in electrochemical performance can be ascribed to the discrepancy in kinetics, wherein ether-based electrolytes exhibit a higher rate of Na+ storage and shedding compared to ester-based electrolytes. This work suggests an effective way to develop doubly doped carbon anode materials for SIBs.

5.
Chemphyschem ; 25(14): e202400341, 2024 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-38878294

RESUMO

Despite prenol emerging as a next-generation biofuel, some questions about its mechanism still need to be adequately proposed to rationalize its consumption and evaluate its efficiency in spark-ignition (SI) engines. Here, we present new insights into the reaction mechanism of prenol (3-methyl-2-buten-1-ol) with OH radicals as a function of temperature and pressure. We have determined that the different temperature and pressure conditions control the preferred products. At combustion temperatures and low pressures, OH-addition adducts are suppressed, increasing the formation of α and δ allylic radicals responsible for the auto-ignition.

6.
Chemphyschem ; 25(11): e202400066, 2024 Jun 03.
Artigo em Inglês | MEDLINE | ID: mdl-38470129

RESUMO

The thermodynamic data on ibuprofen available in the literature shows that the disarray of experimental results is unacceptable for this very important drug. The data on ibuprofens available in the literature were collected, combined with our complementary experimental results and evaluated. The enthalpies of combustion and formation of the crystalline RS-(±)- and S-(+)-ibuprofens were measured using high-precision combustion calorimetry. The temperature dependence of the vapour pressure of S-(+)-ibuprofen was measured using the transpiration method and the enthalpy of vaporization was derived from this measurement. The enthalpies of fusion of both compounds were measured using DSC. The G4 calculations have been carried out to determine the enthalpy of formation in the gaseous state of the most stable conformer. Thermochemical properties of the compounds studied were evaluated and tested for consistency with the "centerpiece approach". A set of reliable and consistent values of thermodynamic properties of ibuprofens at 298.15 K is recommended for thermochemical calculations of the pharmaceutical processes. The diagnostic protocol was developed to distinguish between the "sick" or "healthy" thermodynamic data. This diagnostic is also applicable to other drugs with a different structure than ibuprofen.


Assuntos
Ibuprofeno , Teoria Quântica , Termodinâmica , Ibuprofeno/química , Temperatura , Anti-Inflamatórios não Esteroides/química
7.
Environ Sci Technol ; 58(23): 10357-10367, 2024 Jun 11.
Artigo em Inglês | MEDLINE | ID: mdl-38728016

RESUMO

The urgent environmental concern of methane abatement, attributed to its high global warming potential, necessitates the development of methane oxidation catalysts (MOC) with enhanced low-temperature activity and durability. Herein, an iridium-doped PdOx nanoparticle supported on silicalite-1 zeolite (PdIr/S-1) catalyst was synthesized and applied for methane catalytic combustion. Comprehensive characterizations confirmed the atomically dispersed nature of iridium on the surface of PdOx nanoparticles, creating an Ir4f-O-Pdcus microstructure. The atomically doped Ir transferred more electrons to adjacent oxygen atoms, modifying the electronic structure of PdOx and thus enhancing the redox ability of the PdIr/S-1 catalysts. This electronic modulation facilitated methane adsorption on the Pd site of Ir4f-O-Pdcus, reducing the energy barrier for C-H bond cleavage and thereby increasing the reaction rate for methane oxidation. Consequently, the optimized PdIr0.1/S-1 showed outstanding low-temperature activity for methane combustion (T50 = 276 °C) after aging and maintained long-term stability over 100 h under simulated exhaust conditions. Remarkably, the novel PdIr0.1/S-1 catalyst demonstrated significantly enhanced activity even after undergoing harsh hydrothermal aging at 750 °C for 16 h, significantly outperforming the conventional Pd/Al2O3 catalyst. This work provides valuable insights for designing efficient and durable MOC catalysts, addressing the critical issue of methane abatement.


Assuntos
Irídio , Metano , Nanopartículas , Oxirredução , Metano/química , Irídio/química , Catálise , Nanopartículas/química , Zeolitas/química , Paládio/química
8.
Environ Sci Technol ; 58(25): 11118-11127, 2024 Jun 25.
Artigo em Inglês | MEDLINE | ID: mdl-38864774

RESUMO

Intermediate volatility organic compounds (IVOCs) are important precursors to secondary organic aerosols (SOAs), but they are often neglected in studies concerning SOA formation. This study addresses the significant issue of IVOCs emissions in the Qinghai-Tibetan plateau (QTP), where solid fuels are extensively used under incomplete combustion conditions for residential heating and cooking. Our field measurement data revealed an emission factor of the total IVOCs (EFIVOCs) ranging from 1.56 ± 0.03 to 9.97 ± 3.22 g/kg from various combustion scenarios in QTP. The markedly higher EFIVOCs in QTP than in plain regions can be attributed to oxygen-deficient conditions. IVOCs were dominated by gaseous phase emissions, and the primary contributors of gaseous and particulate phase IVOCs are the unresolved complex mixture and alkanes, respectively. Total IVOCs emissions during the heating and nonheating seasons in QTP were estimated to be 31.7 ± 13.8 and 6.87 ± 0.45 Gg, respectively. The estimated SOA production resulting from combined emissions of IVOCs and VOCs is nearly five times higher than that derived from VOCs alone. Results from this study emphasized the pivotal role of IVOCs emissions in air pollution and provided a foundation for compiling emission inventories related to solid fuel combustion and developing pollution prevention strategies.


Assuntos
Aerossóis , Poluentes Atmosféricos , Carvão Mineral , Compostos Orgânicos Voláteis , Compostos Orgânicos Voláteis/análise , Poluentes Atmosféricos/análise , China , Animais , Tibet , Monitoramento Ambiental
9.
Environ Sci Technol ; 58(8): 3629-3640, 2024 Feb 27.
Artigo em Inglês | MEDLINE | ID: mdl-38354315

RESUMO

Key stages in people's lives have particular relevance for their health; the life-course approach stresses the importance of these stages. Here, we applied a life-course approach to analyze the health risks associated with PM2.5-bound elements, which were measured at three sites with varying environmental conditions in eastern China. Road traffic was found to be the primary source of PM2.5-bound elements at all three locations, but coal combustion was identified as the most important factor to induce both cancer risk (CR) and noncancer risk (NCR) across all age groups due to the higher toxicity of elements such as As and Pb associated with coal. Nearly half of NCR and over 90% of CR occurred in childhood (1-6 years) and adulthood (>18 years), respectively, and females have slightly higher NCR and lower CR than males. Rural population is found to be subject to the highest health risks. Synthesizing previous relevant studies and nationwide PM2.5 concentration measurements, we reveal ubiquitous and large urban-rural environmental exposure disparities over China.


Assuntos
Poluentes Atmosféricos , Material Particulado , Masculino , Feminino , Humanos , Material Particulado/análise , Poluentes Atmosféricos/análise , Estações do Ano , Monitoramento Ambiental , Medição de Risco , China/epidemiologia , Carvão Mineral/análise
10.
Environ Sci Technol ; 58(9): 4268-4280, 2024 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-38393751

RESUMO

Sub-Saharan Africa is a hotspot for biomass burning (BB)-derived carbonaceous aerosols, including light-absorbing organic (brown) carbon (BrC). However, the chemically complex nature of BrC in BB aerosols from this region is not fully understood. We generated smoke in a chamber through smoldering combustion of common sub-Saharan African biomass fuels (hardwoods, cow dung, savanna grass, and leaves). We quantified aethalometer-based, real-time light-absorption properties of BrC-containing organic-rich BB aerosols, accounting for variations in wavelength, fuel type, relative humidity, and photochemical aging conditions. In filter samples collected from the chamber and Botswana in the winter, we identified 182 BrC species, classified into lignin pyrolysis products, nitroaromatics, coumarins, stilbenes, and flavonoids. Using an extensive set of standards, we determined species-specific mass and emission factors. Our analysis revealed a linear relationship between the combined BrC species contribution to chamber-measured BB aerosol mass (0.4-14%) and the mass-absorption cross-section at 370 nm (0.2-2.2 m2 g-1). Hierarchical clustering resolved key molecular-level components from the BrC matrix, with photochemically aged emissions from leaf and cow-dung burning showing BrC fingerprints similar to those found in Botswana aerosols. These quantitative findings could potentially help refine climate model predictions, aid in source apportionment, and inform effective air quality management policies for human health and the global climate.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Humanos , Idoso , Carbono , Biomassa , Monitoramento Ambiental , Poluição do Ar/análise , Aerossóis/análise , Poluentes Atmosféricos/análise , Material Particulado/análise
11.
Environ Sci Technol ; 58(16): 7020-7031, 2024 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-38608167

RESUMO

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.

12.
Environ Sci Technol ; 2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-38323898

RESUMO

The U.S. EPA MOVES3 model was used to assess the impact of the large-scale introduction of electric vehicles on emissions of criteria pollutants (CO, hydrocarbons [HC], NOx, and particulate matter [PM]) and CO2 from the U.S. light-duty vehicle fleet. Large reductions in emissions of these criteria pollutants occurred in 2000-2020. These trends are expected to continue through 2040 driven by turnover of the conventional fleet with old vehicles being replaced by battery electric vehicles (BEVs) and by new internal combustion engine vehicles (ICEVs) with modern emission control systems. Without the introduction of BEVs, the absolute emissions of CO, NOx, HC, and PM2.5 from the U.S. light-duty vehicle fleet are expected to decrease by approximately 61, 88, 55, and 20% from 2020 to 2040. Introduction of BEVs with market share increasing linearly to 100% in 2040 provides additional benefits, which, combined with ICEV fleet turnover, would lead to decreases of absolute emissions of CO, NOx, HC, and PM2.5 of approximately 77, 94, 71, and 37% from 2020 to 2040. Reductions in CO2 emissions follow a similar pattern. Large decreases in criteria pollutant and CO2 emissions from light duty vehicles lie ahead.

13.
Environ Sci Technol ; 58(5): 2458-2467, 2024 Feb 06.
Artigo em Inglês | MEDLINE | ID: mdl-38270113

RESUMO

High-resolution mass spectrometry (HRMS)-based suspect and nontarget screening has identified a growing number of novel per- and polyfluoroalkyl substances (PFASs) in the environment. However, without analytical standards, the fraction of overall PFAS exposure accounted for by these suspects remains ambiguous. Fortunately, recent developments in ionization efficiency (IE) prediction using machine learning offer the possibility to quantify suspects lacking analytical standards. In the present work, a gradient boosted tree-based model for predicting log IE in negative mode was trained and then validated using 33 PFAS standards. The root-mean-square errors were 0.79 (for the entire test set) and 0.29 (for the 7 PFASs in the test set) log IE units. Thereafter, the model was applied to samples of liver from pilot whales (n = 5; East Greenland) and white beaked dolphins (n = 5, West Greenland; n = 3, Sweden) which contained a significant fraction (up to 70%) of unidentified organofluorine and 35 unquantified suspect PFASs (confidence level 2-4). IE-based quantification reduced the fraction of unidentified extractable organofluorine to 0-27%, demonstrating the utility of the method for closing the fluorine mass balance in the absence of analytical standards.


Assuntos
Fluorocarbonos , Poluentes Químicos da Água , Animais , Fluorocarbonos/análise , Poluentes Químicos da Água/análise , Espectrometria de Massas , Flúor , Mamíferos
14.
J Pharmacol Sci ; 154(2): 86-96, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38246732

RESUMO

Heated tobacco products (HTPs) are marketed worldwide as less harmful alternatives to combustible cigarettes; however, their cytotoxic mechanisms in vascular smooth muscle cells are poorly understood. Ferroptosis is defined as iron-dependent cell death caused by the accumulation of lipid peroxidation products. In this study, the cytotoxic effects of nicotine- and tar-free cigarette smoke extracts (CSE) derived from three types of HTPs and the ferroptosis inducer, erastin, on vascular smooth muscle A7r5 cells were compared. Cigarette smoke from all HTPs was generated according to the following puffing regime: 55 mL, puff volume; 30 s, puff interval; 2 s, puff duration; bell-shaped, puff profile; and no blocking of the ventilation holes. Erastin and CSE decreased mitochondrial metabolic activity and increased lactate dehydrogenase leakage. The cytotoxic effects of erastin were almost completely inhibited by the radical-trapping antioxidant, UAMC-3203; iron chelator, deferoxamine mesylate (DFO); 12/15-lipoxygenase (12/15-LOX) inhibitor, baicalein; and selective 15-LOX inhibitor, ML351. In contrast, CSE-induced cell damage was partially attenuated by UAMC-3203, baicalein, and ML351 but not by DFO. These results suggest that erastin induces ferroptosis via 15-LOX-mediated iron-dependent lipid peroxidation, whereas CSE causes iron-independent cell damage via 15-LOX-mediated lipid peroxidation-dependent and -independent mechanisms.


Assuntos
Antineoplásicos , Fumar Cigarros , Ferroptose , Piperazinas , Produtos do Tabaco , Músculo Liso Vascular , Ferro
15.
J Fluoresc ; 34(1): 397-409, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37278962

RESUMO

In the present system, Sm3+ activated Ba2BiV3O11 nanomaterial series radiating orange-red light was developed via an efficient approach of solution combustion method. The structural examinations using XRD analysis indicate that the sample is crystallized into the monoclinic phase with the P21/a (14) space group. The elemental composition and morphological conduct were studied via energy dispersive spectroscopy (EDS) and scanning electron microscopy (SEM) respectively. Also, the formation of nanoparticles was confirmed by transmission electron microscopy (TEM). Photoluminescent (PL) examinations reveal the orange-red emission from the developed nanocrystals via documenting the emission spectra, which reveals the peak at 606 nm due to the 4G5/2 → 6H7/2 transition. Further, the decay time, non-radiative rates, quantum efficiency, and band gap of the optimal sample were computed as 1.3263 ms, 219.5 s- 1, 70.88%, and 3.41 eV respectively. Finally, the chromatic parameters including color - coordinates (0.5565, 0.4426), 1975 K color correlated temperature (CCT), and color purity (85.58%) reflected their excellent luminous performance. The above-mentioned outcomes endorsed the relevancy of the developed nanomaterials as a propitious agent in the engineering of advanced illuminating optoelectronic appliances.

16.
J Fluoresc ; 2024 Aug 17.
Artigo em Inglês | MEDLINE | ID: mdl-39153166

RESUMO

Solution combustion procedure was used to create a succession of Na3LaxSm1 - x(PO4)2 (x = 0.01-0.15 mol) nanocrystals that generate a warm deep reddish light. Both HR-TEM and X-ray diffraction examinations were used to examine the morphology and crystalline phase analysis. Energy-dispersive X-ray analysis (EDAX) approves the elemental examination. The luminescence spectrum exhibits a decent reddish-orange emission at 700 nm wavelength upon near-UV illumination, which aligns with the electronic transition 4G5/2 → 6H11/2. According to Dexter's idea, nearest neighbor interlinkages are responsible for the concentration quenching that occurs after the Sm3+ ion composition reaches 6 mol%. Additionally, a detailed evaluation of the radiative lifespan (0.7519 ms), quantum efficiency (77%), Non radiative rate (307.40), color temperature (3170 K), color purity (99.2%) and color coordinates (0.652, 0.338) was conducted. The optical characteristics that have been observed indicate that Sm3+ doped Na3La(PO4)2 phosphors could be a good option for improving WLED efficiency and color quality.

17.
J Fluoresc ; 34(2): 627-633, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-37338724

RESUMO

The combustion procedure was used to synthesize Bi2Al4O9:Eu3+ phosphors. The XRD and photoluminescence properties are investigations. The XRD patterns consist of an orthorhombic crystal structure. At 395 nm, the maximum excitation intensity was obtained. Following 395 nm excitation, two different emission peaks at 593 and 615 nm were observed. Concentration quenching occurred at 0.5 mol % Eu3+ ions. The CIE coordinates for the Bi2Al4O9 phosphor with Eu3+ ion doped are 615 nm (x = 0.680, y = 0.319) falling in the red region. According to the photoluminescence results, Bi2Al4O9:Eu3+ phosphors might be useful in the fields of near UV-excited w-LEDs.

18.
Anal Bioanal Chem ; 2024 Aug 19.
Artigo em Inglês | MEDLINE | ID: mdl-39160436

RESUMO

Carbon-13 isotopomics of triacylglycerol (TAG) fatty acids or free fatty acids in biological matrices holds considerable potential in food authentication, forensic investigations, metabolic studies, and medical research. However, challenges arise in the isotopic analysis of short- and medium-chain (C4 to C10) fatty acid methyl esters (SMCFAMEs) through gas chromatography-combustion-isotope ratio mass spectrometry (GC-C-IRMS). The high volatility of these esters results in losses during their preparation, leading to isotopic fractionation. Moreover, the methoxy group added to acyl chains requires the correction of δ13C values, thereby increasing the uncertainty of the final results. Analyzing free fatty acids (FFAs) addresses both issues encountered with SMCFAMEs. To achieve this objective, we have developed a new protocol enabling the isotopomics of individual fatty acids (FAs) by GC-C-IRMS. The same experiment also provides the FA profile, i.e., the relative percentage of each FA in the TAG hydrolysate or its concentration in the studied matrix. The method exhibited high precision, as evidenced by the repeatability and within-lab reproducibility of results when tested on TAGs from both animal and vegetal origins. Compared to the analysis of FAMEs by GC-C-IRMS, the current procedure also brings several improvements in alignment with the principles of green analytical chemistry and green sample preparation. Thus, we present a two-in-one method for 13C-isotopomic and metabolomic biomarker quantitation within quasi-universal TAG compounds, encompassing the short- and medium-acyl chains.

19.
Anal Bioanal Chem ; 416(11): 2859-2870, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38459967

RESUMO

Microwave-induced combustion (MIC) was proposed in this study for honey decomposition aiming for As, Cd, Hg, and Pb determination by inductively coupled plasma mass spectrometry (ICP-MS). Sample mass (up to 1.0 g), absorbing solution (0.5 to 14.4 mol L-1 HNO3, and H2O), heating program, and combustion aids were evaluated. The Eurachem guidelines were used for method validation. The proposed method enabled combustion of a high sample mass (0.8 g of honey, with 0.4 g of microcrystalline cellulose and 100 µL of 6 mol L-1 NH4NO3) using 6 mL of an absorbing solution consisting of 1 mol L-1 HNO3, which resulted in low residual carbon in solution (< 25 mg L-1). Honey samples from different geographical origins were analyzed. Results showed no significant difference in comparison to other two microwave decomposition methods, based on microwave-assisted wet digestion with single reaction chamber (MAWD-SRC) and microwave-assisted wet digestion (MAWD). Standard addition experiments resulted in recoveries higher than 98%. The limits of detection ranged from 1.10 (As) to 4.60 ng g-1 (Pb). In addition to using only diluted reagents and resulting in digests virtually free of interferences, the proposed method was faster (< 30 min) than most of those presented in the literature.


Assuntos
Mel , Micro-Ondas , Espectrometria de Massas/métodos , Chumbo , Análise Espectral
20.
Environ Res ; 243: 117734, 2024 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-38029827

RESUMO

Under the influence of human activities, atmospheric mercury (Hg) concentrations have increased by 450% compared with natural levels. In the context of the Minamata Convention on Mercury, which came into effect in August 2017, it is imperative to strengthen Hg emission controls. Existing Air Pollution Control Devices (APCDs) combined with collaborative control technology can effectively remove Hg2+ and Hgp; however, Hg0 removal is substandard. Compared with the catalytic oxidation method, Hg0 removal through adsorbent injection carries the risk of secondary release and is uneconomical. Magnetic adsorbents exhibit excellent recycling and Hg0 recovery performance and have recently attracted the attention of researchers. This review summarizes the existing magnetic materials for Hg0 adsorption and discusses the removal performances and mechanisms of iron, carbon, mineral-based, and magnetosphere materials. The effects of temperature and different flue gas components, including O2, NO, SO2, H2O, and HCl, on the adsorption performance of Hg0 are also summarized. Finally, different regeneration methods are discussed in detail. Although the research and development of magnetic adsorbents has progressed, significant challenges remain regarding their application. This review provides theoretical guidance for the improvement of existing and development of new magnetic adsorbents.


Assuntos
Poluentes Atmosféricos , Mercúrio , Humanos , Poluentes Atmosféricos/análise , Mercúrio/análise , Oxirredução , Fenômenos Magnéticos , Carvão Mineral , Centrais Elétricas
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