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1.
J Hazard Mater ; 475: 134795, 2024 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-38878427

RESUMEN

Functionalization of graphene enables precise control over interlayer spacing during film formation, thereby enhancing the separation efficiency of radioactive ions in graphene membranes. However, the systematic impact of interlayer spacing of graphene membranes on radioactive-ion separation remains unexplored. This study aims to elucidate how interlayer spacing in functionalized graphene membranes affects the separation of radioactive ions. Utilizing polyamidoxime (PAO) to modify graphene oxide, we controlled the interlayer spacing of graphene membranes. Experimental results indicate that tuning interlayer spacing enables control of the permeation flux of radioactive ions (UO22+ 1.01 × 10-5-8.32 × 10-5 mol/m2·h, and K+ remains stable at 3.60 × 10-4 mol/m2·h), and the K+/UO22+ separation factors up to 36.2 at an interlayer spacing of 8.8 Å. Using density functional theory and molecular dynamics simulations, we discovered that the effective separation is mainly determined via interlayer spacing and the quantity of introduced functional groups, explaining the anomalous high permeation flux of target ions at low interlayer spacing (4.3 Å). This study deepens our comprehension of interlayer spacing within nanoconfined spaces for ion separation and recovery via graphene membranes, offering valuable insights for the design and synthesis of high-performance nanomembrane materials.

2.
Sci Total Environ ; 917: 170298, 2024 Mar 20.
Artículo en Inglés | MEDLINE | ID: mdl-38272098

RESUMEN

Microplastics, as an emerging pollutant, are widely distributed worldwide. Extensive research has been conducted to address the issue of microplastic pollution; however, effective methods for microplastic treatment are still lacking. This study innovatively utilizes electron beam technology to age and degrade microplastics. Compared to other treatment methods, electron beam technology can effectively promote the aging and degradation of microplastics. The Oxygen - carbon ratio of aged microplastics reached 0.071, with a mass loss of 48 % and a carbonyl index value of 0.69, making it the most effective method for short-term aging treatment in current research efforts. Theoretical calculations and experimental results demonstrate that a large number of oxygen-containing functional groups are generated on the surface of microplastics after electron beam irradiation, changing their adsorption performance for pollutants. Theoretical calculations show that an increase in oxygen-containing functional groups on the surface leads to a gradual decrease in hydrophobic pollutant adsorption capacity while increasing hydrophilic pollutant adsorption capacity for aged microplastics. Experimental studies were conducted to investigate the adsorption behavior and process of typical pollutants by aged microplastics which conform to pseudo-second-order kinetics and Henry model during the adsorption process, and the adsorption results are consistent with theoretical calculations. The results show that the degradation of microplastics is mainly due to hydroxyl radicals generated by electron beam irradiation, which can break the carbon chain of microplastics and gradually degrade them into small molecular esters and alcohols. Furthermore, studies have shown that microplastics can desorb pollutants in pure water and simulated gastric fluid. Overall, electron beam irradiation is currently the most effective method for degrading microplastics. These results also clearly elucidate the characteristics and mechanisms of the interaction between aged microplastics and organic pollutants, providing further insights for assessing microplastic pollution in real-world environments.

3.
Chemosphere ; 318: 137939, 2023 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-36702419

RESUMEN

With the increasing incidence and mortality of cardiovascular diseases, high consumption of the cardiovascular drug salbutamol (SAL) has made this compound an emerging pollutant in natural water and a challenge for traditional wastewater treatment. In this paper, an efficient advanced oxidation process was used to degrade SAL by electron beam (EB) irradiation. The results revealed that 100 mg L-1 of SAL could be nearly completely removed (95.1%) at 10 kGy and the degradation kinetic well followed pseudo first-order kinetic model. Different factors, including pH, inorganic ions and water matrix, had varying effects on the degradation of SAL owing to their important influence on the formation of reactive species in the aqueous solution. And it was found that eaq- played a major role in the degradation of SAL parent. Moreover, the addition of K2S2O8 (20 mM) increased the SAL mineralization rate from 2.9% to 64.2%, suggesting that oxidation free radicals could greatly improve the mineralization rate of SAL. Combining with the theoretical calculations and determined degradation by-products, four possible degradation pathways of SAL by EB irradiation were proposed, including H•, •OH and eaq- all participated in the degradation of SAL. Finally, toxicity evaluation suggested that the toxicity of SAL aqueous solution reduced after EB irradiation, indicating that it is an effective method to degrade SAL.


Asunto(s)
Contaminantes Químicos del Agua , Purificación del Agua , Albuterol , Electrones , Oxidación-Reducción , Agua , Contaminantes Químicos del Agua/análisis , Purificación del Agua/métodos , Cinética
4.
Chemosphere ; 336: 138992, 2023 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-37271473

RESUMEN

Heavy metals (HMs) and polycyclic aromatic hydrocarbons (PAHs) in industrial wastewater have attracted much attention due to their damage to the environment and the human body. Studies have shown that there may be interactions between PAHs and HMs, leading to enhanced toxicity of both pollutants. It has been shown that traditional methods are difficult to treat a combination of PAHs and HMs simultaneously. This paper presented an innovative method for treating PAHs and HMs compound pollutants by electron beam irradiation and achieved the removal of the compound pollutants using a single means. Experiments showed that the absorbed dose at 15 kGy could achieve 100% degradation of NAP and 90% reduction of Cr (Ⅵ). This article investigated the effects of electron beam removal of PAHs and HMs complex contaminants in various water environmental matrices. The experimental results showed that the degradation of NAP followed the pseudo-first-order dynamics, and the degradation of NAP was more favorable under neutral conditions. Inorganic ions and water quality had little effect on NAP degradation. For electron beam reduction of Cr (Ⅵ), alkaline conditions were more conducive to reducing Cr (Ⅵ). Especially, adding K2S2O8 or HCOOH achieved 99% reduction of Cr (Ⅵ). Experiments showed that •OH achieve the degradation of NAP, and eaq- achieve the reduction of Cr (Ⅵ). The results showed that the degradation of NAP was mainly achieved by benzene ring opening, carboxylation and aldehyde, which proved that the degradation of NAP was mainly caused by •OH attack. The toxicity analysis results showed that the electron beam could significantly reduce the toxicity of NAP, and the toxicity of the final product was much lower than NAP, realizing the harmless treatment of NAP. The experimental results showed that electron beam irradiation has faster degradation rates and higher degradation efficiency for NAP and Cr (Ⅵ) compared to other reported treatment methods.


Asunto(s)
Contaminantes Ambientales , Metales Pesados , Hidrocarburos Policíclicos Aromáticos , Humanos , Electrones , Naftalenos , Hidrocarburos Policíclicos Aromáticos/análisis
5.
Chemosphere ; 303(Pt 2): 134964, 2022 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-35609661

RESUMEN

Benzothiazole (BTH) is a typical refractory heterocyclic compound that can be used as a photosensitive material in organic synthesis and conditional plant resource research. The extensive use of BTH has led to high BTH concentrations in natural environment, such as in tap water and urine, which tend to inhibit animal hormone synthesis and induce genotoxicity. Traditional wastewater treatment processes cannot effectively remove BTH. Therefore, we aimed to use the electron beam method, an emerging method for pollutant degradation, to degrade BTH in water. Experiments showed that BTH can be effectively degraded (up to 90%) when the electron beam reaches 5 kGy and irradiation conformed perfectly to the pseudo first-order kinetics model. Experimental results showed that acidic conditions are more favorable for electron beam degradation of BTH, while the degradation of most other inorganic ions is inhibited (except SO42-). Hydroxyl radicals (•OH) was confirmed to play a major role in degradation by the experiment, and the mineralization rate was greatly increased by the addition of H2O2 and K2S2O8. In addition, our experimental and theoretical calculations showed that the degradation of BTH occurred mainly through the opening of the benzene ring. Theoretical calculations showed that the toxicity of BTH decreased significantly after electron beam degradation, making it an effective way to degrade BTH.


Asunto(s)
Peróxido de Hidrógeno , Contaminantes Químicos del Agua , Animales , Benzotiazoles , Electrones , Cinética , Oxidación-Reducción , Agua , Contaminantes Químicos del Agua/análisis
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