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1.
J Hazard Mater ; 439: 129622, 2022 10 05.
Artigo em Inglês | MEDLINE | ID: mdl-35868082

RESUMO

Removal and recovery of uranium from uranium-mine wastewater is beneficial to environmental protection and resource preservation. Reduction of soluble hexavalent U (U(VI)) to insoluble tetravalent uranium (U(IV)) by microbes is a plausible approach for this purpose, but its practical implementation has long been restricted by its intrinsic drawbacks. The electro-stimulated microbial process offers promise in overcoming these drawbacks. However, its applicability in real wastewater has not been evaluated yet, and its U(VI) removal mechanisms remain poorly understood. Herein, we report that introducing a weak electro-stimulation considerably boosted microbial U(VI) removal activities in both synthetic and real wastewater. The U(VI) removal has proceeded via U(VI)-to-U(IV) reduction in the biocathode, and the electrochemical characterization demonstrates the crucial role of the electroactive biofilm. Microbial community analysis shows that the broad biodiversity of the cathode biofilm is capable of U(VI) reduction, and the molecular ecological network indicates that synthetic metabolisms among electroactive and metal-reducing bacteria play major roles in electro-microbial-mediated uranium removal. Metagenomic sequencing elucidates that the electro-stimulated U(VI) bioreduction may proceed via e-pili, extracellular electron shuttles, periplasmic and outer membrane cytochrome, and thioredoxin pathways. These findings reveal the potential and mechanism of the electro-stimulated U(VI) bioreduction system for the treatment of U-bearing wastewater.


Assuntos
Urânio , Poluentes Radioativos da Água , Bactérias/metabolismo , Biodegradação Ambiental , Oxirredução , Urânio/química , Águas Residuárias , Poluentes Radioativos da Água/química
2.
J Hazard Mater ; 432: 128723, 2022 06 15.
Artigo em Inglês | MEDLINE | ID: mdl-35316632

RESUMO

Removing and recovering uranium (U) from U-mining wastewater would be appealing, which simultaneously reduces the adverse environmental impact of U mining activities and mitigates the depletion of conventional U resources. In this study, we demonstrate the application of a constant-voltage electrochemical (CVE) method for the removal and recovery of U from U-mining wastewater, in an ambient atmosphere. The effects of operation conditions were elucidated in synthetic U-bearing water experiments, and the cell voltage and the ionic strength were found to play important roles in both the U extraction kinetics and the operation cost. The mechanistic studies show that, in synthetic U-bearing water, the CVE U extraction proceeds exclusively via a single-step one-electron reduction mechanism, where pentavalent U is the end product. In real U-mining wastewater, the interference of water matrices led to the disproportionation of the pentavalent U, resulting in the formation of tetravalent and hexavalent U in the extraction products. The U extraction efficacy of the CVE method was evaluated in real U-mining wastewater, and results show that the CVE U extraction method can be efficient with operation costs ranging from $0.55/kgU ~ $64.65/kgU, with varying cell voltages from 1.0 V to 4.0 V, implying its feasibility from the economic perspective.


Assuntos
Urânio , Poluentes Radioativos da Água , Mineração , Águas Residuárias , Água , Poluentes Radioativos da Água/análise
3.
Sci Total Environ ; 804: 150218, 2022 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-34798744

RESUMO

In this study, knowledge gaps on Sb concentration in rocks, ores, tailings, soil, river water, sediments, and crops of mine areas were identified and discussed in terms of contamination levels, spatial distribution, and environmental effects. Accordingly, Xunyang Hg-Sb mine, the largest Hg-Sb deposit in China as research region in this study, field sampling and laboratory analysis were conducted. The results showed elevated concentrations of Sb in the soil, sediment, and river water. The X-ray diffraction analysis indicated that the main minerals of the rocks were quartz, dolomite, calcite, and margarite. Based on the TESCAN integrated mineral analyzer analysis, the main ore minerals in the Gongguan mine were dolomite (93.97%), cinnabar (2.50%), stibnite (2.48%), calcite (0.38%), and quartz (0.38%). The µ-XRF analysis indicated that Sb distribution was similar to those of S and O, instead of those of Hg and As. The clear spatial variation of Sb concentration in environmental media, mines, tailings, and settling ponds affected Sb accumulation. Actinobacteriota, Proteobacteria, Acidobacteriota, and Chloroflexi were the dominant phyla in the soil. Patescibacteria, Proteobacteria, and Bdellovibrionota were negatively correlated with Sb in the soil (p < 0.05). Exposure to Sb through maize grain and cabbage consumption poses serious non-carcinogenic health risk for residents. This work provides a scientific basis for the environmental quality assessment of Sb mine areas and development of applicable guidelines.


Assuntos
Mercúrio , Poluentes do Solo , Antimônio/análise , China , Monitoramento Ambiental , Mercúrio/análise , Mineração , Solo , Poluentes do Solo/análise
4.
iScience ; 24(11): 103230, 2021 Nov 19.
Artigo em Inglês | MEDLINE | ID: mdl-34712926

RESUMO

Current photocatalytic uranium (U) extraction methods have intrinsic obstacles, such as the recombination of charge carriers, and the deactivation of catalysts by extracted U. Here we show that, by applying a bias potential on the photocatalyst, the photoelectrochemical (PEC) method can address these limitations. We demonstrate that, owing to efficient spatial charge-carriers separation driven by the applied bias, the PEC method enables efficient and durable U extraction. The effects of multiple operation conditions are investigated. The U extraction proceeds via single-step one-electron reduction, resulting in the formation of pentavalent U, which can facilitate future studies on this often-overlooked U species. In real seepage water the PEC method achieves an extraction capacity of 0.67 gU m-3·h-1 without deactivation for 156 h continuous operation, which is 17 times faster than the photocatalytic method. This work provides an alternative tool for U resource recovery and facilitates future studies on U(V) chemistry.

5.
J Org Chem ; 86(19): 13734-13743, 2021 10 01.
Artigo em Inglês | MEDLINE | ID: mdl-34541847

RESUMO

An efficient, facile, and eco-friendly synthesis of pyrimidine derivatives has been developed. It involves a [3 + 2 + 1] three-component annulation of amidines, ketones, and one carbon source. N,N-Dimethylaminoethanol is oxidized through C(sp3)-H activation to provide the carbon donor. One C-C and two C-N bonds are formed during the oxidative annulation process. The reaction shows good tolerance to many important functional groups in air, making this methodology a highly versatile alternative, and significant improvement to the existing methods for structuring a pyrimidine framework, especially 4-aliphatic pyrimidines.


Assuntos
Amidinas , Cetonas , Carbono , Catálise , Deanol , Pirimidinas
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