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1.
Environ Geochem Health ; 46(8): 297, 2024 Jul 09.
Article in English | MEDLINE | ID: mdl-38980451

ABSTRACT

The radiological characterization of soil contaminated with natural radionuclides enables the classification of the area under investigation, the optimization of laboratory measurements, and informed decision-making on potential site remediation. Neural networks (NN) are emerging as a new candidate for performing these tasks as an alternative to conventional geostatistical tools such as Co-Kriging. This study demonstrates the implementation of a NN for estimating radiological values such as ambient dose equivalent (H*(10)), surface activity and activity concentrations of natural radionuclides present in a waste dump of a Cu mine with a high level of natural radionuclides. The results obtained using a NN were compared with those estimated by Co-Kriging. Both models reproduced field measurements equivalently as a function of spatial coordinates. Similarly, the deviations from the reference concentration values obtained in the output layer of the NN were smaller than the deviations obtained from the multiple regression analysis (MRA), as indicated by the results of the root mean square error. Finally, the method validation showed that the estimation of radiological parameters based on their spatial coordinates faithfully reproduced the affected area. The estimation of the activity concentrations was less accurate for both the NN and MRA; however, both methods gave statistically comparable results for activity concentrations obtained by gamma spectrometry (Student's t-test and Fisher's F-test).


Subject(s)
Copper , Mining , Neural Networks, Computer , Radiation Monitoring , Soil Pollutants, Radioactive , Copper/analysis , Soil Pollutants, Radioactive/analysis , Radiation Monitoring/methods , Regression Analysis
2.
J Contam Hydrol ; 265: 104392, 2024 Jun 26.
Article in English | MEDLINE | ID: mdl-38954926

ABSTRACT

More than 60% of worldwide uranium production is based on the In Situ Recovery mining technique. This exploitation method directly falls within the scope of the applications of reactive transport modelling to optimize uranium production and limit its associated environmental impact. We propose a modelling approach which is able to represent the natural evolution of an aquifer impacted by an ISR test performed using sulfuric acid. The model is calibrated on a 12 year-long data series obtained from 12 monitoring wells surrounding an ISR pilot cell. Through this process-based approach, we simulate the impact of several remediation strategies that can be considered in these contexts. In particular, we model the impact of Pump & Treat combined with reverse osmosis, as well as the circulation of non-impacted fluids through the reservoir with different operating strategies. Our approach allows to compare the effectiveness of these strategies. For this small-scale ISR pilot, monitored natural attenuation constitutes an interesting approach due to its faster pH recovery time with respect to Pump & Treat (5-10 years to pH ∼ 6), whose efficiency can be improved by the addition of exchangeable cations. Circulation of unimpacted fluids can reduce pH recovery times if performed for periods longer than the ISR exploitation and/or deployed with a delay. Combined with an economic evaluation of their deployment, this modelling approach can help the mining operator select and design optimal remediation strategies from an environmental and economical standpoint.

3.
Adv Sci (Weinh) ; : e2404397, 2024 Jul 01.
Article in English | MEDLINE | ID: mdl-38946685

ABSTRACT

Extraction of U(VI) in water is of great significance in energy and environmental fields. However, the traditional methods usually fail due to the indispensable extra addition of catalyst, adsorbent, precipitant, or sacrificial agents, which may lead to enhanced extraction costs and secondary pollution. Here, a new efficient uranium extraction strategy is proposed based on triboelectricity without adding a catalyst or other additives. It is found only under the friction between the microbubbles (generated under ultrasonication) and the water flow, that reactive oxygen species (ROS) can largely be generated, which thus contributes to the solidification of U(VI) from water. In addition, the magnetic field can affect the phase of the product. Under mechanical stirring, the product contains (UO2)O2·2H2O, while which contains UO2(OH)2 and (UO2)O2·4H2O under the magnetic stirring. Quenching experiments are also carried out to explore the influence of environmental factors. Most importantly, it shows great potential in the extraction of U(VI) from seawater. This work proposes a catalyst-free and light-free strategy toward the solidification of U(VI) from water, which avoids the secondary pollution of the catalyst to the environment and is low-cost, and has great potential in the real application.

4.
Sci Total Environ ; : 174406, 2024 Jul 02.
Article in English | MEDLINE | ID: mdl-38964395

ABSTRACT

The remediation of groundwater subject to in situ leaching (ISL) for uranium mining has raised extensive concerns in uranium mill and milling. This study conducted bioremediation through biostimulation and bioaugmentation to the groundwater in an area in northern China that was contaminated due to uranium mining using the CO2 + O2 neutral ISL (NISL) technology. It identified the dominant controlling factors and mechanisms driving bioremediation. Findings indicate that microorganisms can reduce the uranium concentration in groundwater subject to NISL uranium mining to its normal level. After 120 days of bioaugmentation, the uranium concentration in the contaminated groundwater fell to 0.36 mg/L, achieving a remediation efficiency of 91.26 %. Compared with biostimulation, bioaugmentation shortened the remediation timeframe by 30 to 60 days while maintaining roughly the same remediation efficiency. For groundwater remediation using indigenous microbial inoculants, initial uranium concentration and low temperatures (below 15 °C) emerge as the dominant factors influencing the bioremediation performance and duration. In settings with high carbonate concentrations, bioremediation involved the coupling of multiple processes including bioreduction, biotransformation, biomineralization, and biosorption, with bioreduction assuming a predominant role. Post-bioremediation, the relative abundances of reducing microbes Desulfosporosinus and Sulfurospirillum in groundwater increased significantly by 10.56 % and 6.91 %, respectively, offering a sustainable, stable biological foundation for further bioremediation of groundwater.

5.
Article in English | MEDLINE | ID: mdl-38961273

ABSTRACT

BACKGROUND: American Indian (AI) communities are affected by uranium exposure from abandoned mines and naturally contaminated drinking water. Few studies have evaluated geographical differences across AI communities and the role of dietary exposures. OBJECTIVE: We evaluated differences in urinary uranium levels by diet and geographical area among AI participants from the Northern Plains, the Southern Plains, and the Southwest enrolled in the Strong Heart Family Study (SHFS). METHODS: We used food frequency questionnaires to determine dietary sources related to urinary uranium levels for 1,682 SHFS participants in 2001-2003. We calculated adjusted geometric mean ratios (GMRs) of urinary uranium for an interquartile range (IQR) increase in self-reported food group consumption accounting for family clustering and adjusting for sociodemographic variables and other food groups. We determined the percentage of variability in urinary uranium explained by diet. RESULTS: Median (IQR) urinary uranium levels were 0.027 (0.012, 0.057) µg/g creatinine. Urinary uranium levels were higher in Arizona (median 0.039 µg/g) and North Dakota and South Dakota (median 0.038 µg/g) and lower in Oklahoma (median 0.019 µg/g). The adjusted percent increase (95% confidence interval) of urinary uranium levels per IQR increase in reported food intake was 20% (5%, 36%) for organ meat, 11% (1%, 23%) for cereals, and 14% (1%, 29%) for alcoholic drinks. In analyses stratified by study center, the association with organ meat was specific to North Dakota and South Dakota participants. An IQR increase in consumption of fries and chips was inversely associated with urinary uranium levels -11% (-19%, -3%). Overall, we estimated that self-reported dietary exposures explained 1.71% of variability in urine uranium levels. IMPACT: Our paper provides a novel assessment of self-reported food intake and urinary uranium levels in a cohort of American Indian participants. We identify foods (organ meat, cereals, and alcohol) positively associated with urinary uranium levels, find that organ meat consumption is only associated with urine uranium in North Dakota and South Dakota, and estimate that diet explains relatively little variation in total urinary uranium concentrations. Our findings contribute meaningful data toward a more comprehensive estimation of uranium exposure among Native American communities and support the need for high-quality assessments of water and dust uranium exposures in SHFS communities.

6.
Environ Technol ; : 1-9, 2024 Jul 04.
Article in English | MEDLINE | ID: mdl-38962999

ABSTRACT

Immobilisation of uranium (U (VI)) by direct precipitation of uranyl phosphate (U-P) exhibits a great potential application in the remediation of U (VI)-contaminated environments. However, phosphorus, vital element of bacteria's decomposition, absorption and transformationmay affect the stability of U (VI) with ageing time. The main purpose of this work is to study the effect of bacteria on uranium sequestration mechanism and stability by different forms of phosphorus in a water sedimentary system. The results showed that phosphate effectively enhanced the removal of U (VI), with 99.84%. X-Ray Diffraction (XRD), Scanning Electron Microscopy and Energy Dispersive Spectrometer (SEM-EDS), and X-ray Photoelectron Spectroscopy (XPS) analyses imply that U (VI) and U (IV) co-exist on the surface of the samples. Combined with BCR results, it demonstrated that bacteria and phosphorus have a synergistic effect on the removal of U (VI), realising the immobilisation of U (VI) from a transferable phase to a stable phase. However, from a long-term perspective, the redissolution and release of uranium immobilisation of U (VI) by pure bacteria with ageing time are worthy of attention, especially in uranium mining environments rich in sensitive substances. This observation implies that the stability of the uranium may be impacted by the prevailing environmental conditions. The novel findings could provide theoretical evidence for U (VI) bio-immobilisation in U (VI)-contaminated environments.

7.
Chemosphere ; : 142742, 2024 Jul 04.
Article in English | MEDLINE | ID: mdl-38971441

ABSTRACT

Uranium (U) is a chemical and radioactive toxic contaminant affecting many groundwater systems. The focus of this study was to evaluate the suitability of forward osmosis (FO) for uranium rejection from contaminated groundwater under field-relevant conditions. Laboratory experiments with aqueous solution containing uranium were performed with FO membrane to understand the uranium rejection mechanism under varied pH, draw solution concentration, and presence of co-ions. Further, experiments were performed with U-contaminated field groundwater. Results of the hydrogeochemcial modelling using PHREEQC indicated that the rejection mechanism of uranium was highly dependent on aqueous speciation. Uranium rejection was maximum at alkaline pH with ca. 99% rejection due to charge-based interactions between membrane and dominant uranyl complexes. The results of the co-ion study indicated that nitrate and phosphate ions decrease uranium rejection. Whereas, bicarbonates, calcium, and magnesium ions concentrated uranium in feed solution. Further, the uranium adsorption onto the membrane surface primarily depended on pH of the aqueous solution with maximum adsorption at pH 5.5. Our results show that the World Health Organization's drinking water guideline value of 30 µgL-1 for U could be achieved via FO process in field groundwater containing low dissolved solids.

8.
J Contam Hydrol ; 265: 104390, 2024 Jun 29.
Article in English | MEDLINE | ID: mdl-38959822

ABSTRACT

Uranium mainly comes from ISL of sandstone-type uranium deposits in China. The change of porosity and permeability caused by blockage of ore-bearing strata is one of the most serious problems in acid ISL of uranium. In this paper, the groundwater tracer test was carried out before and 1 year after ISL to explore the pore and permeability evolution characteristics of the ore-bearing layer during ISL. The test results showed that the leaching solution migrated along two seepage channels and the water-bearing medium was isotropic. After 1 year of ISL, the flow rate of the leaching solution decreased obviously. However, the flow rate of the leaching solution in slower channel decreased more than that in the faster channel in all directions, which was caused by the more adequate chemical reactions between the leaching solution and the minerals of the ore-bearing layer and the more corresponding precipitation in the slower channel. In addition, the flow rate along the direction of groundwater flow decreased less than that in the direction of vertical groundwater flow. This was closely related to the transformation of aquifer medium by hydrodynamic field. Initial stage of ISL, the occurrence of plugging is closely related to the precipitation-dissolution process of iron and aluminum minerals under the change of pH, which is accompanied by the continuous precipitation of gypsum.

9.
J Environ Radioact ; 278: 107469, 2024 Jun 17.
Article in English | MEDLINE | ID: mdl-38889474

ABSTRACT

Compacted soil layers effectively prevent the migration of radon gas from uranium tailings impoundments to the nearby environment. However, surface damage caused by wet and dry cycles (WDCs) weakens this phenomenon.In order to study the effect of crack network on radon exhalation under WDCs, a homemade uranium tailing pond model was developed to carry out radon exhalation tests under five WDCs. Based on image processing and morphological methods, the area, length, mean width and fractal dimension of the drying cracks were quantitatively analyzed, and multiple linear regression was used to establish the relationship between the geometric characteristics of the cracks and the radon exhalation rate under multiple WDCs. The results suggested that the radon release rate and crack network of the uranium tailings pond gradually stabilized as the water content decreased, following rapid development in a single WDC process. The radon release rate increased continuously after each cycle, with a cumulative increase of 25.9% over 5 cycles. The radon release rate and average crack width remained consistent in size, and a binary linear regression considering width and fractal dimension could explain the changes in radon release rate after multiple WDCs.

10.
Water Res ; 260: 121912, 2024 Jun 08.
Article in English | MEDLINE | ID: mdl-38875858

ABSTRACT

Numerous investigations have illuminated the profound impact of phosphate on the adsorption of uranium, however, the effect of phosphate-mediated surface modification on the reactivity of zero-valent iron (ZVI) remained enigmatic. In this study, a phosphate-modified ZVI (P-ZVIbm) was prepared with a facile ball milling strategy, and compared with ZVIbm, the U(VI) removal amount (435.2 mg/g) and efficiency (3.52×10-3 g·mg-1·min-1) of P-ZVIbm were disclosed nearly 2.0 and 54 times larger than those of ZVIbm respectively. The identification of products revealed that the adsorption mechanism dominated the removal process for ZVIbm, while the reactive modified layer strengthened both the adsorption pattern and reduction performance on P-ZVIbm. DFT calculation result demonstrated that the binding configuration shifted from bidentate binuclear to multidentate configuration, further shortening the Fe-U atomic distance. More importantly, the electron transferred is more accessible through the surface phosphate layer, and selectively donated to U(VI), accounting for the elevated reduction performance of P-ZVIbm. This investigation explicitly underscores the critical role of ZVI's surface microenvironment in the domain of radioactive metal ion mitigation and introduces a novel methodology to amplify the sequestration of U(VI) from aqueous environments.

11.
Chemosphere ; 361: 142544, 2024 Aug.
Article in English | MEDLINE | ID: mdl-38844100

ABSTRACT

Nuclear energy is playing an increasingly important role on the earth, but the nuclear plants leaves a legacy of radioactive waste pollution, especially uranium-containing pollution. Straw biochar with wide sources, large output, low cost, and easy availability, has emerged as a promising material for uranium extraction from radioactive wastewater, but the natural biomass with suboptimal structure and low content of functional groups limits the efficiency. In this work, microbial etch was first came up to regulate the biochar's structure and function. The surface of the biochar becomes rougher and more microporous, and the mineral contents (Ca, P) indirectly increased by microbial etch. The biochar was modified by calcium phosphate and exhibited a remarkable uranium extraction capacity of 590.8 mg g-1 (fitted value). This work provides a cost-effective and sustainable method for preparing functionalized biochar via microbial etch, which has potential for application to uranium extraction from radioactive wastewater.


Subject(s)
Charcoal , Uranium , Wastewater , Charcoal/chemistry , Uranium/chemistry , Wastewater/chemistry , Radioactive Waste/analysis , Water Pollutants, Radioactive , Calcium Phosphates/chemistry
12.
Sci Total Environ ; 942: 173755, 2024 Sep 10.
Article in English | MEDLINE | ID: mdl-38851336

ABSTRACT

In order to realize the low-carbon development policy, the large-scale development and utilization of nuclear energy is very essential. Uranium is the key resource for nuclear industry. The extracting and recycling uranium from seawater and nuclear wastewater is necessary for secure uranium reserves, ensure energy security, control pollution and protect the environment. The novel nanomaterial MXene possesses the layered structure, high specific surface area, and modifiable surface terminal groups, which allowed it to enrich uranium. In addition, good photovoltaic and photothermal properties improves the ability to adsorb uranium. The excellent radiation resistance of the MAX phase strongly indicates the potential use of MXene as an effective uranium adsorbent. However, there are relatively few reviews on its application in uranium extraction and recovery. This review focuses on the recent advances in the use of MXene-based materials as highly efficient adsorbents for the recovery of uranium from seawater and nuclear wastewater. First, the structural, synthetic and characterization aspects of MXene materials are introduced. Subsequently, the adsorptive properties of MXene-based materials are evaluated in terms of uranium extraction recovery capability, selectivity, and reproducibility. Furthermore, the interaction mechanisms between uranium and MXene absorbers are discussed. Finally, the challenges for MXene materials in uranium adsorption applications are proposed for better design of new types of MXene-based adsorbents.

13.
J Hazard Mater ; 476: 134975, 2024 Jun 19.
Article in English | MEDLINE | ID: mdl-38908177

ABSTRACT

Phosphate-solubilizing bacteria (PSB) are important but often overlooked regulators of uranium (U) cycling in soil. However, the impact of PSB on uranate fixation coupled with the decomposition of recalcitrant phosphorus (P) in mining land remains poorly understood. Here, we combined gene amplicon sequencing, metagenome and metatranscriptome sequencing analysis and strain isolation to explore the effects of PSB on the stabilization of uranate and P availability in U mining areas. We found that the content of available phosphorus (AP), carbonate-U and Fe-Mn-U oxides in tailings was significantly (P < 0.05) higher than their adjacent soils. Also, organic phosphate mineralizing (PhoD) bacteria (e.g., Streptomyces) and inorganic phosphate solubilizing (gcd) bacteria (e.g., Rhodococcus) were enriched in tailings and soils, but only organic phosphate mineralizing-bacteria substantially contributed to the AP. Notably, most genes involved in organophosphorus mineralization and uranate resistance were widely present in tailings rather than soil. Comparative genomics analyses supported that organophosphorus mineralizing-Streptomyces species could increase soil AP content and immobilize U(VI) through organophosphorus mineralization (e.g., PhoD, ugpBAEC) and U resistance related genes (e.g., petA). We further demonstrated that the isolated Streptomyces sp. PSBY1 could enhance the U(VI) immobilization mediated by the NADH-dependent ubiquinol-cytochrome c reductase (petA) through decomposing organophosphorous compounds. This study advances our understanding of the roles of PSB in regulating the fixation of uranate and P availability in U tailings.

14.
Small ; : e2402847, 2024 Jun 07.
Article in English | MEDLINE | ID: mdl-38845471

ABSTRACT

A large amount of radioactive waste is accumulated in the process of nuclear fuel preparation, causing serious pollution to the environment and abundant depleted uranium resources to be abandoned. One of the key issues affecting the development of nuclear energy is how to make full use of depleted uranium resources efficiently. Here, U element with unique coordination mode of 5f electron is spacer bonded to transition metal with 3d orbit through the adsorption and anchoring effect of MXene, thus U and Co dual doped MXene catalyst is constructed along with the comprehensive utilization of depleted uranium resources. The as-prepared U-Co/MXene catalyst demonstrates excellent overpotential of only 184 mV at -10 mA cm-2 and excellent stability up to 150 h, significantly surpassing the bare MXene substrate. Theoretical calculations indicate that the U and Co dual doping optimizes the electronic structure of MXene catalyst by forming the U-O-Co network, thereby improving the thermodynamics of H* adsorption during the catalytic transition state. This research opens up a new path for the recovery of depleted uranium resources and the development of functional actinide catalysts.

15.
J Hazard Mater ; 475: 134869, 2024 Aug 15.
Article in English | MEDLINE | ID: mdl-38870857

ABSTRACT

Photoreduction of highly toxic U(VI) to less toxic U(IV) is crucial for mitigating radioactive contamination. Herein, a CoWO4/TpDD p-n heterojunction is synthesized, with TpDD serving as the n-type semiconductor substrate and CoWO4 as the p-type semiconductor grown in situ on its surface. The Fermi energy difference between TpDD and CoWO4 provides the electrochemical potential for charge-hole separation. Moreover, the Coulombic forces from the distinct carrier types between the two materials synergistically facilitate the transfer of electrons and holes. Hence, an internal electric field directed from TpDD to CoWO4 is established. Under photoexcitation conditions, charges and holes migrate efficiently along the curved band and internal electric field, further enhancing charge-hole separation. As a result, the removal capacity of CoWO4/TpDD increases from 515.2 mg/g in the dark to 1754.6 mg/g under light conditions. Thus, constructing a p-n heterojunction proves to be an effective strategy for remediating uranium-contaminated environments.

16.
J Hazard Mater ; 476: 135044, 2024 Jun 26.
Article in English | MEDLINE | ID: mdl-38943881

ABSTRACT

Deep geological repositories (DGRs) stand out as one of the optimal options for managing high-level radioactive waste (HLW) such as uranium (U) in the near future. Here, we provide novel insights into microbial behavior in the DGR bentonite barrier, addressing potential worst-case scenarios such as waste leakage (e.g., U) and groundwater infiltration of electron rich donors in the bentonite. After a three-year anaerobic incubation, Illumina sequencing results revealed a bacterial diversity dominated by anaerobic and spore-forming microorganisms mainly from the phylum Firmicutes. Highly U tolerant and viable bacterial isolates from the genera Peribacillus, Bacillus, and some SRB such as Desulfovibrio and Desulfosporosinus, were enriched from U-amended bentonite. The results obtained by XPS and XRD showed that U was present as U(VI) and as U(IV) species. Regarding U(VI), we have identified biogenic U(VI) phosphates, U(UO2)·(PO4)2, located in the inner part of the bacterial cell membranes in addition to U(VI)-adsorbed to clays such as montmorillonite. Biogenic U(IV) species as uraninite may be produced as result of bacterial enzymatic U(VI) reduction. These findings suggest that under electron donor-rich water-saturation conditions, bentonite microbial community can control U speciation, immobilizing it, and thus enhancing future DGR safety if container rupture and waste leakage occurs.

17.
Chemosphere ; 362: 142667, 2024 Jun 19.
Article in English | MEDLINE | ID: mdl-38906190

ABSTRACT

This study presents the successful synthesis of Magnesium-aluminum layered double hydroxide composite phosphate-modified hydrothermal biochar for efficient removal of U(VI) from aqueous solutions. A novel synthesis approach involving phosphate thermal polymerization-hydrothermal method was employed, deviating from conventional pyrolysis methods, to produce hydrothermal biochar. The combination of solvent thermal polymerization technique with hydrothermal process facilitated efficient loading of layered double hydroxide (LDH) components onto the biochar surface, ensuring simplicity, low energy consumption and enhanced modifiability. Bamboo waste was utilized as the precursor for biochar, highlighting its superior green and sustainable characteristics. Additionally, this study elucidated the interactions between phosphate-modified hydrothermal biochar and LDH components with U(VI). Physicochemical analysis demonstrated that the composite biochar possessed a high surface area and abundant oxygen-containing functional groups. XPS and FTIR analyses confirmed the efficient adsorption of U(VI), attributed to chelation interactions between phosphate groups, magnesium hydroxyl groups, hydroxyl groups and U(VI), as well as the co-precipitation of U(VI) with multi-hydroxyl aluminum cations captured by LDH. The composite biochar reached adsorption equilibrium with U(VI) within 80 min and exhibited excellent fitting to the pseudo-second-order kinetic model and Langmuir model. Under conditions of pH = 4 and 298 K, it displayed significantly high maximum adsorption capacity of approximately 388.81 mg g⁻1, surpassing untreated biochar by 17-fold. The adsorption process was found to be endothermic and spontaneous and even after five consecutive adsorption-desorption cycles, the removal efficiency of U(VI) remained stable at 75.46%. These findings underscore the promising application prospects of Magnesium-aluminum layered double hydroxide composite phosphate-modified hydrothermal biochar in efficiently separating U(VI) from uranium-containing wastewater, emphasizing its environmental and economic value.

18.
J Mol Model ; 30(7): 216, 2024 Jun 18.
Article in English | MEDLINE | ID: mdl-38888814

ABSTRACT

CONTEXT: The efficient extraction of uranyl from spent nuclear fuel wastewater for subsequent reprocessing and reuse is an essential effort toward minimization of long-lived radioactive waste. N-substituted amides and Schiff base ligands are propitious candidates, where extraction occurs via complexation with the uranyl moiety. In this study, we extensively probed chemical bonding in various uranyl complexes, utilizing the local vibrational modes theory alongside QTAIM and NBO analyses. We focused on (i) the assessment of the equatorial O-U and N-U bonding, including the question of chelation, and (ii) how the strength of the axial U = O bonds of the uranyl moiety changes upon complexation. Our results reveal that the strength of the equatorial uranium-ligand interactions correlates with their covalent character and with charge donation from O and N lone pairs into the vacant uranium orbitals. We also found an inverse relationship between the covalent character of the equatorial ligand bonds and the strength of the axial uranium-oxygen bond. In summary, our study provides valuable data for a strategic modulation of N-substituted amide and Schiff base ligands towards the maximization of uranyl extraction. METHOD: Quantum chemistry calculations were performed under the PBE0 level of theory, paired with the relativistic NESCau Hamiltonian, currently implemented in Cologne2020 (interfaced with Gaussian16). Wave functions were expanded in the cc-pwCVTZ-X2C basis set for uranium and Dunning's cc-pVTZ for the remaining atoms. For the bonding properties, we utilized the package LModeA in the local modes analyses, AIMALL in the QTAIM calculations, and NBO 7.0 for the NBO analyses.

19.
Int J Biol Macromol ; 272(Pt 1): 132776, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38823750

ABSTRACT

Uranium as a nuclear fuel, its source and aftertreatment has been a hot topic of debate for developers. In this paper, amidoxime and guanidino-modified cotton fibers (DC-AO-PHMG) were synthesized by the two-step functionalization approach, which exhibited remarkable antimicrobial and high uranium recovery property. Adsorption tests revealed that DC-AO-PHMG had excellent selectivity and anti-interference properties, the maximum adsorption capacity of 609.75 mg/g. More than 85 % adsorption capacity could still be kept after 10 adsorption-desorption cycles, and it conformed to the pseudo-second-order kinetic model and the Langmuir adsorption isotherm model as a spontaneous heat-absorbing chemical monolayer process. FT-IR, EDS and XPS analyses speculated that the amidoxime and amino synergistically increased the uranium uptake. The inhibitory activities of DC-AO-PHMG against three aquatic bacteria, BEY, BEL (from Yellow River water and lake bottom silt, respectively) and B. subtilis were significantly stronger, and the uranium adsorption was not impacted by the high bacteria content. Most importantly, DC-AO-PHMG removed up to 94 % of uranium in simulated seawater and extracted up to 4.65 mg/g of uranium from Salt Lake water, which demonstrated its great potential in the field of uranium resource recovery.


Subject(s)
Cotton Fiber , Oximes , Uranium , Uranium/chemistry , Adsorption , Oximes/chemistry , Sewage/chemistry , Sewage/microbiology , Kinetics , Anti-Bacterial Agents/pharmacology , Anti-Bacterial Agents/chemistry , Water Purification/methods
20.
Carbohydr Polym ; 339: 122283, 2024 Sep 01.
Article in English | MEDLINE | ID: mdl-38823934

ABSTRACT

Efficient removal of uranium from radioactive wastewater is crucial for both environmental protection and sustainable development of nuclear energy. However, selectively extracting uranium from acidic wastewater remains a significant challenge. Here we present a phytic acid-functionalized polyamidoxime/alginate hydrogel (PAG) via a facile one-step hydrothermal reaction. The PAG, leveraging the robust binding affinity of phytic acid and the selective coordination of amidoxime for U(VI), exhibited high efficiency and selectivity in adsorbing U(VI) from acidic uranium-containing wastewater. At pH 2.50, U(VI) adsorption equilibrium was achieved within 60 min, showcasing a maximum theoretical adsorption capacity of 218.34 mg/g. Additionally, the PAG demonstrated excellent reusability, maintaining a uranium removal rate exceeding 90 % over five adsorption-desorption cycles. Remarkably, the as-synthesized PAG removed 94.1 % of U(VI) from actual acidic uranium-contaminated groundwater with excellent anti-interference performance, reducing U(VI) concentration from 272.0 µg/L to 16.1 µg/L and making it meet the WHO drinking water standards (30 µg/L). The adsorption mechanism was elucidated through XPS and DFT calculation, revealing that the uranyl ion primarily coordinated with phosphate and amidoxime groups on phytic acid and polyamidoxime, respectively. These findings underscore the promising potential of PAG hydrogel for addressing acidic uranium-containing wastewater from uranium mining and metallurgy.

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