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1.
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
2.
Int J Biol Macromol ; 273(Pt 1): 132780, 2024 Jul.
Article in English | MEDLINE | ID: mdl-38825291

ABSTRACT

Manufacturing a highly effective sorbent for removing UO22+ ions from aqueous effluents is vital for safeguarding the environment and recovering valuable resources. This research presents an innovative strategy employing adsorbents derived from pullulan, specifically tailored with furfuryl-amidoxime (FAO), to improve their affinity for UO22+ ions. The formation of a UO22+ ion-imprinted sorbent (U-II-P) was achieved by crosslinking the UO22+/FAO-modified pullulan (FAO-P) complex with bis(maleimido)ethane (BME) via click Diels-Alder (DA) cyclization, enhancing its attraction and specificity for UO22+ ions. Detailed characterization of the synthesis was performed using NMR and FTIR spectroscopy, and the sorbent's external textures were analyzed using scanning electron microscopy (SEM). The U-II-P sorbent showcased outstanding preference for UO22+ over other metallic ions, with the most efficient adsorption occurring at pH 5. It exhibited a significant adsorption capacity of 262 mg/g, closely aligning with the predictions of the Langmuir adsorption model and obeying pseudo-second-order kinetic behavior. This investigation underlines the effectiveness of FAO-P as a specialized solution for UO22+ ion extraction from wastewater, positioning it as a viable option for the remediation of heavy metals.


Subject(s)
Glucans , Oximes , Uranium , Glucans/chemistry , Oximes/chemistry , Uranium/chemistry , Adsorption , Click Chemistry/methods , Kinetics , Water Pollutants, Chemical/chemistry , Water Pollutants, Chemical/isolation & purification , Water Purification/methods , Hydrogen-Ion Concentration , Ions/chemistry
3.
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
4.
World J Microbiol Biotechnol ; 40(7): 232, 2024 Jun 05.
Article in English | MEDLINE | ID: mdl-38834810

ABSTRACT

Microbially induced carbonate precipitation (MICP) has been used to cure rare earth slags (RES) containing radionuclides (e.g. Th and U) and heavy metals with favorable results. However, the role of microbial extracellular polymeric substances (EPS) in MICP curing RES remains unclear. In this study, the EPS of Lysinibacillus sphaericus K-1 was extracted for the experiments of adsorption, inducing calcium carbonate (CaCO3) precipitation and curing of RES. The role of EPS in in MICP curing RES and stabilizing radionuclides and heavy metals was analyzed by evaluating the concentration and morphological distribution of radionuclides and heavy metals, and the compressive strength of the cured body. The results indicate that the adsorption efficiencies of EPS for Th (IV), U (VI), Cu2+, Pb2+, Zn2+, and Cd2+ were 44.83%, 45.83%, 53.7%, 61.3%, 42.1%, and 77.85%, respectively. The addition of EPS solution resulted in the formation of nanoscale spherical particles on the microorganism surface, which could act as an accumulating skeleton to facilitate the formation of CaCO3. After adding 20 mL of EPS solution during the curing process (Treat group), the maximum unconfined compressive strength (UCS) of the cured body reached 1.922 MPa, which was 12.13% higher than the CK group. The contents of exchangeable Th (IV) and U (VI) in the cured bodies of the Treat group decreased by 3.35% and 4.93%, respectively, compared with the CK group. Therefore, EPS enhances the effect of MICP curing RES and reduces the potential environmental problems that may be caused by radionuclides and heavy metals during the long-term sequestration of RES.


Subject(s)
Bacillaceae , Calcium Carbonate , Extracellular Polymeric Substance Matrix , Metals, Heavy , Thorium , Uranium , Uranium/chemistry , Uranium/metabolism , Calcium Carbonate/chemistry , Thorium/chemistry , Extracellular Polymeric Substance Matrix/metabolism , Extracellular Polymeric Substance Matrix/chemistry , Bacillaceae/metabolism , Metals, Rare Earth/chemistry , Adsorption , Chemical Precipitation
5.
Water Res ; 258: 121817, 2024 Jul 01.
Article in English | MEDLINE | ID: mdl-38810598

ABSTRACT

Electrochemical uranium extraction (EUE) from seawater is a very promising strategy, but its practical application is hindered by the high potential for electrochemical system, as well as the low selectivity, efficiency, and poor stability of electrode. Herein, we developed creatively a low potential strategy for persistent uranium recovery by electrochemistry-assisted in-situ regeneration of oxygen vacancies and Ti(III) active sites coupled with indirect reduction of uranium, finally achieving high selectivity, efficient and persistent uranium recovery. As-designed titanium dioxide rich in oxygen vacancies (TiO2-VO) electrode displayed an EUE efficiency of ∼99.9 % within 180 min at a low potential of 0.09 V in simulated seawater with uranium of 5∼20 ppm. Moreover, the TiO2-VO electrode also showed high selectivity (89.9 %) to uranium, long-term cycling stability and antifouling activity in natural seawater. The excellent EUE property was attributed to the fact that electrochemistry-assisted in-situ regeneration of oxygen vacancies and Ti(III) active sites enhanced EUE cycling process and achieved persistent uranium recovery. The continuous regeneration of oxygen vacancies not only reduced the adsorption energy of U(VI)O22+ but also serve as a storage and transportation channel for electrons, accelerating electron transfer from Ti(III) to U(VI) at solid-liquid interface and promoting EUE kinetic rate.


Subject(s)
Oxygen , Seawater , Titanium , Uranium , Uranium/chemistry , Titanium/chemistry , Oxygen/chemistry , Seawater/chemistry , Electrodes , Electrochemistry , Electrochemical Techniques , Water Pollutants, Radioactive/chemistry
6.
Environ Pollut ; 352: 124062, 2024 Jul 01.
Article in English | MEDLINE | ID: mdl-38701963

ABSTRACT

The leaching process of uranium tailings is a typical water-rock interaction. The release of 226Ra from uranium tailings depends on the nuclides outside the intrinsic properties of uranium tailings on the one hand, and is influenced by the water medium on the other. In this paper, a uranium tailings repository in southern China was used as a research object, and uranium tailings at different depths were collected by drilling samples and mixed to analyze the 226Ra occurrence states. Static dissolution leaching experiments of 226Ra under different pH conditions, solid-liquid ratio conditions, and ionic strength conditions were carried out, and the adsorption and desorption behaviours of 226Ra in five representative stratigraphic media were investigated. The results show that 226Ra has a strong adsorption capacity in representative strata, with adsorption distribution coefficient Kd values ranging from 1.07E+02 to 1.29E+03 (mL/g) and desorption distribution coefficients ranging from 4.97E+02 to 2.71E+03 (mL/g), but the adsorption is reversible. The 226Ra in uranium tailings exists mainly in the residual and water-soluble states, and the release of 226Ra from uranium tailings under different conditions is mainly from the water-soluble and exchangeable state fractions. Low pH conditions, low solid-liquid ratio conditions and high ionic strength conditions are favourable to the release of 226Ra from uranium tailings, so the release of 226Ra from uranium tailings can be reduced by means of adjusting the pH in the tailings and setting up a water barrier. The results of this research have important guiding significance for the management of existing uranium tailings ponds and the control of 226Ra migration in groundwater, which is conducive to guaranteeing the long-term safety, stability and sustainability of uranium mining sites.


Subject(s)
Radium , Uranium , Uranium/chemistry , Adsorption , Radium/analysis , Radium/chemistry , China , Soil Pollutants, Radioactive/analysis , Radiation Monitoring , Mining , Water Pollutants, Radioactive/chemistry , Water Pollutants, Radioactive/analysis
7.
Mikrochim Acta ; 191(6): 302, 2024 05 06.
Article in English | MEDLINE | ID: mdl-38709346

ABSTRACT

A sensitive and biocompatible N-rich probe for rapid visual uranium detection was constructed by grafting two trianiline groups to 2,6-bis(aminomethyl)pyridine. Possessing excellent aggregation-induced emission (AIE) property and the advantages to form multidentate chelate with U selectively, the probe has been applied successfully to visualize uranium in complex environmental water samples and living cells, demonstrating outstanding anti-interference ability against large equivalent of different ions over a wide effective pH range. A large linear range (1.0 × 10-7-9.0 × 10-7 mol/L) and low detection limit (72.6 nmol/L, 17.28 ppb) were achieved for the visual determination of uranium. The recognition mechanism, photophysical properties, analytical performance and cytotoxicity were systematically investigated, demonstrating high potential for fast risk assessment of uranium pollution in field and in vivo.


Subject(s)
Fluorescent Dyes , Uranium , Uranium/analysis , Uranium/chemistry , Fluorescent Dyes/chemistry , Fluorescent Dyes/toxicity , Humans , Limit of Detection , Biocompatible Materials/chemistry , HeLa Cells , Cell Survival/drug effects , Optical Imaging , Aniline Compounds/chemistry , Aniline Compounds/toxicity , Pyridines/chemistry
8.
Int J Biol Macromol ; 270(Pt 2): 132491, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38763240

ABSTRACT

Capacitive deionization (CDI) technology holds great potential for rapid and efficient uranyl ion removal from wastewater. However, the related electrode materials still have much room for research. Herein, chitosan/phytic acid complexes were anchored on polypyrrole nanotubes (CS/PA-PPy) to fabricate the electrode for the electrosorption of uranyl ions (UO22+). In this system, polypyrrole nanotubes provided specific channels for ion and electron diffusion, and chitosan/phytic acid complexes offered selective sites for UO22+ binding. The results demonstrated that CS/PA-PPy via electrosorption showed faster kinetics and higher uranium uptake than those via physicochemical adsorption. The maximum adsorption capacity toward UO22+ via electrosorption (1.2 V) could reach 799.3 mg g-1, which was higher than most of the reported CDI electrodes. Electrochemical measurements and experimental characterizations showed that the electrosorption of UO22+ by CS/PA-PPy was a synergistic effect of capacitive process and physicochemical adsorption, in which the capacitive mechanism involved the formation of an electric double layer from hollow polypyrrole nanotubes, whereas the coordination of phosphate, amino and hydroxyl groups with UO22+ was attributed to physicochemical adsorption. With the rational design of material, along with its excellent uranium removal performance, this work exhibited a novel and potential composite electrode for uranium capture via CDI from wastewater.


Subject(s)
Chitosan , Electrodes , Nanotubes , Polymers , Pyrroles , Uranium , Wastewater , Uranium/chemistry , Uranium/isolation & purification , Polymers/chemistry , Wastewater/chemistry , Pyrroles/chemistry , Nanotubes/chemistry , Adsorption , Chitosan/chemistry , Water Purification/methods , Kinetics
9.
Environ Sci Technol ; 58(21): 9456-9465, 2024 May 28.
Article in English | MEDLINE | ID: mdl-38745405

ABSTRACT

The elimination of uranium from radioactive wastewater is crucial for the safe management and operation of environmental remediation. Here, we present a layered vanadate with high acid/base stability, [Me2NH2]V3O7, as an excellent ion exchanger capturing uranyl from highly complex aqueous solutions. The material possesses an indirect band gap, ferromagnetic characteristic and a flower-like morphology comprising parallel nanosheets. The layered structure of [Me2NH2]V3O7 is predominantly upheld by the H-bond interaction between anionic framework [V3O7]nn- and intercalated [Me2NH2]+. The [Me2NH2]+ within [Me2NH2]V3O7 can be readily exchanged with UO22+. [Me2NH2]V3O7 exhibits high exchange capacity (qm = 176.19 mg/g), fast kinetics (within 15 min), high removal efficiencies (>99%), and good selectivity against an excess of interfering ions. It also displays activity for UO22+ ion exchange over a wide pH range (2.00-7.12). More importantly, [Me2NH2]V3O7 has the capability to effectively remove low-concentration uranium, yielding a residual U concentration of 13 ppb, which falls below the EPA-defined acceptable limit of 30 ppb in typical drinking water. [Me2NH2]V3O7 can also efficiently separate UO22+ from Cs+ or Sr2+ achieving the highest separation factors (SFU/Cs of 589 and SFU/Sr of 227) to date. The BOMD and DFT calculations reveal that the driving force of ion exchange is dominated by the interaction between UO22+ and [V3O7]nn-, whereas the ion exchange rate is influenced by the mobility of UO22+ and [Me2NH2]+. Our experimental findings indicate that [Me2NH2]V3O7 can be considered as a promising uranium scavenger for environmental remediation. Additionally, the simulation results provide valuable mechanistic interpretations for ion exchange and serve as a reference for designing novel ion exchangers.


Subject(s)
Uranium , Vanadates , Uranium/chemistry , Vanadates/chemistry , Ion Exchange , Water Pollutants, Radioactive/chemistry , Kinetics
10.
Water Res ; 257: 121683, 2024 Jun 15.
Article in English | MEDLINE | ID: mdl-38703542

ABSTRACT

Efficient uranium capture from wastewater holds great importance for the environmental remediation and sustainable development of nuclear energy, but it is a tremendous challenge. Herein, a facile and scalable approach is reported to fabricate functionalized hierarchical porous polymers (PPN-3) decorated with high density of phosphate groups for uranium adsorption. The as-constructed hierarchical porous structure could allow rapid diffusion of uranyl ions, while abundant phosphate groups that serve as adsorption sites could provide the high affinity for uranyl. Consequently, PPN-3 shows a high uranium adsorption uptake of 923.06 mg g-1 and reaches adsorption equilibrium within simply 10 min in uranium-spiked aqueous solution. Moreover, PPN-3 affords selective adsorption of uranyl over multiple metal ions and possesses a rapid and high removal rate of U(VI) in real water systems. Furthermore, this study offers direct polymerization strategy for the cost-effective fabrication of phosphate-functionalized porous organic polymers, which may provide promising application potential for uranium extraction.


Subject(s)
Polymers , Uranium , Uranium/chemistry , Adsorption , Polymers/chemistry , Porosity , Water Purification/methods , Water Pollutants, Radioactive
11.
Int J Biol Macromol ; 267(Pt 2): 131608, 2024 May.
Article in English | MEDLINE | ID: mdl-38621558

ABSTRACT

Amidoxime-based fiber adsorbents hold significant promise for uranium extraction. However, a notable issue is that these adsorbents primarily originate from synthetic polymer materials, which, aside from providing good mechanical support, have no other functions. In recent study, we shifted our focus to silk fiber (SF), a natural protein fiber known for its unique core-shell structure and rich amino acids. The shell layer, due to its abundant functional groups, makes it easily modifiable, while the core layer provides excellent mechanical strength. Leveraging these inherent properties, an amidoxime-based fiber adsorbent was developed. This adsorbent utilizes amino and carboxyl groups for enhanced performance synergistically. This method involves establishing uranium affinity sites on the outer sericin layer of SF via chemical initiation of graft polymerization (CIGP) and amidoximation (SF-g-PAO). The water absorption ratio of SF-g-PAO is as high as 601.16 % (DG = 97.17 %). Besides, SF-g-PAO demonstrates an exceptional adsorption capacity of 15.69 mg/g in simulated seawater, achieving a remarkable removal rate of uranyl ions at 95.06 %. It can withstand a minimum of five adsorption-elution cycles. Over a 4-week period in natural seawater, SF-g-PAO displayed an adsorption capacity of 4.95 mg/g. Furthermore, SF-g-PAO also exhibits impressive uranium removal efficiency in real nuclear wastewater, with a removal rate of 63 % in just 15 min and a final removal rate of 90 %. It is hoped that this SF-g-PAO, prepared through this straightforward method and characterized by the synergistic action of amino and carboxyl groups, can offer innovative insights into the development of uranium extraction adsorbents.


Subject(s)
Oximes , Silk , Uranium , Uranium/chemistry , Adsorption , Oximes/chemistry , Silk/chemistry , Fibroins/chemistry
12.
J Contam Hydrol ; 263: 104343, 2024 04.
Article in English | MEDLINE | ID: mdl-38631090

ABSTRACT

The long-term management of tailings from former uranium (U) mines requires an in-depth understanding of the hydrogeological processes and water flow paths. In France, most of the legacy U mines are located in fractured crystalline (plutonic) rocks, where the intrinsic subsurface heterogeneity adds to the uncertainties about the former extraction and milling activities and the state of the mine when production was ceased. U ores were mainly processed by sulfuric acid leaching, leading to high-sulfate-content mill tailings now contained in several tailing storage facilities (TSFs). The La Ribière site, located in western central France, is a former open-pit and underground U mine, closed in 1992 and used to store mill tailings. This site is being used as a test case to establish a workflow in order to explain and predict water flow and subsurface contaminant transport. A conceptual model of water flow and sulfate transport, at the scale of the La Ribière watershed, is first developed based on available information and hydrogeochemical monitoring. Recent geophysical investigations allows refining this model. Electrical Resistivity Tomography (ERT) proves to be efficient at localizing the extent of the highly conductive sulfate plume inherited from the U-mill tailings, but also at imaging the weathering profile. Magnetic Resonance Sounding (MRS), despite the limited signal intensity due to the low porosity in crystalline rocks, gives some insight into the porosity values, the depth of the fractured layer and the location of the low-porosity ore-processing muds. Based on this conceptual model, a 3D flow and non-reactive transport model with the METIS code is developed and calibrated. This model allows predicting the evolution of the sulfate plume, but will also be used in future investigations, to build reactive transport models with simplified hydrogeology for U and other reactive contaminants.


Subject(s)
Mining , Uranium , Water Movements , Uranium/chemistry , France , Models, Theoretical , Water Pollutants, Radioactive/analysis , Environmental Monitoring/methods , Silicon Dioxide/chemistry , Groundwater/chemistry , Uncertainty , Sulfates/chemistry
13.
Int J Biol Macromol ; 266(Pt 2): 131400, 2024 May.
Article in English | MEDLINE | ID: mdl-38582480

ABSTRACT

The aim of the present research is to fabricate a biosorbent using agricultural waste for removal of uranium from contaminated water i.e. "waste to wealth" approach. Cellulose extracted from wheat straw was mercerized and a novel semi-interpenetrating polymer network (semi-IPN) was fabricated through graft copolymerization of polyvinyl alcohol onto hybrid mercerized cellulose + collagen backbone. Response surface methodology was used for optimization of different reaction parameters as a function of % grafting (195.1 %) was carried out. Semi-IPN was found to possess higher thermal stability. Adsorption results revealed that the optimum parameters for the elimination of uranium using semi-IPN were: adsorbent dose = 0.15 g, pH = 6.0, contact time = 120 min and initial U (VI) concentration = 100 µg/L. The pseudo-second-order kinetic model gave the best description of the adsorption equilibrium data as the calculated qe value is nearest to the experimental qe for the different initial U(VI) concentrations. Adsorption experiments followed Langmuir isotherm with R2 = 0.999. Furthermore, recyclability and reusability studies showed that the adsorption efficiency of semi-IPN was 82 % after 5 cycles indicating the superior recycling execution of fabricated biosorbent. Thus, the fabricated ecofriendly device can be used effectively for the removal of uranium from contaminated wastewater sources.


Subject(s)
Cellulose , Collagen , Uranium , Water Purification , Uranium/chemistry , Cellulose/chemistry , Adsorption , Water Purification/methods , Kinetics , Collagen/chemistry , Hydrogen-Ion Concentration , Water Pollutants, Chemical/chemistry , Water Pollutants, Chemical/isolation & purification , Temperature , Ions/chemistry
14.
Inorg Chem ; 63(16): 7464-7472, 2024 Apr 22.
Article in English | MEDLINE | ID: mdl-38598182

ABSTRACT

Uranium accumulation in the kidneys and bones following internal contamination results in severe damage, emphasizing the pressing need for the discovery of actinide decorporation agents with efficient removal of uranium and low toxicity. In this work, cinnamic acid (3-phenyl-2-propenoic acid, CD), a natural aromatic carboxylic acid, is investigated as a potential uranium decorporation ligand. CD demonstrates markedly lower cytotoxicity than that of diethylenetriaminepentaacetic acid (DTPA), an actinide decorporation agent approved by the FDA, and effectively removes approximately 44.5% of uranyl from NRK-52E cells. More importantly, the results of the prompt administration of the CD solution remove 48.2 and 27.3% of uranyl from the kidneys and femurs of mice, respectively. Assessments of serum renal function reveal the potential of CD to ameliorate uranyl-induced renal injury. Furthermore, the single crystal of CD and uranyl compound (C9H7O2)2·UO2 (denoted as UO2-CD) reveals the formation of uranyl dimers as secondary building units. Thermodynamic analysis of the solution shows that CD coordinates with uranyl to form a 2:1 molar ratio complex at a physiological pH of 7.4. Density functional theory (DFT) calculations further show that CD exhibits a significant 7-fold heightened affinity for uranyl binding in comparison to DTPA.


Subject(s)
Cinnamates , Uranium , Cinnamates/chemistry , Cinnamates/pharmacology , Animals , Ligands , Mice , Uranium/chemistry , Uranium/metabolism , Uranium/toxicity , Kidney/drug effects , Kidney/metabolism , Cell Line , Density Functional Theory , Rats , Molecular Structure , Cell Survival/drug effects , Chelating Agents/chemistry , Chelating Agents/pharmacology , Chelating Agents/chemical synthesis
15.
PLoS One ; 19(4): e0292414, 2024.
Article in English | MEDLINE | ID: mdl-38568898

ABSTRACT

To mitigate the risk of radioactive isotope dissemination, the development of preventative and curative measures is of particular interest. For mass treatment, the developed solution must be easily administered, preferably orally, with effective, nontoxic decorporating properties against a wide range of radioactive isotopes. Currently, most orally administered chelation therapy products are quickly absorbed into the blood circulation, where chelation of the radioactive isotope is a race against time due to the short circulation half-life of the therapeutic. This report presents an alternative therapeutic approach by using a functionalized chitosan (chitosan@DOTAGA) with chelating properties that remains within the gastrointestinal tract and is eliminated in feces, that can protect against ingested radioactive isotopes. The polymer shows important in vitro chelation properties towards different metallic cations of importance, including (Cs(I), Ir(III), Th(IV), Tl(I), Sr(II), U(VI) and Co(II)), at different pH (from 1 to 7) representing the different environments in the gastrointestinal tract. An in vivo proof of concept is presented on a rodent model of uranium contamination following an oral administration of Chitosan@DOTAGA. The polymer partially prevents the accumulation of uranium within the kidneys (providing a protective effect) and completely prevents its uptake by the spleen.


Subject(s)
Chitosan , Radiation-Protective Agents , Uranium , Chitosan/chemistry , Uranium/chemistry , Radiation-Protective Agents/pharmacology , Polymers , Chelating Agents/chemistry
16.
J Environ Radioact ; 276: 107441, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38677042

ABSTRACT

Residues generated from the uranium purification process, characterized by a high uranium content, pose a significant challenge for recovery through leaching and present a considerable environmental threat. After using XRD and SEM-mapping characterization analysis combined with the BCR continuous graded extraction test to analyze the content of different states of uranium, it was found that the main reason why the uranium in the residue was difficult to leach because it was encapsulated by SiO2 crystals. Using NH4HF2 as a leaching agent, a leaching study of uranium in the residue was carried out, and the results showed that the H+ and F- produced by NH4HF2could react with SiO2, destroying the crystal lattice of SiO2 and causing the encapsulated uranium to come into contact with the leaching agent, facilitating the leaching of uranium in the residue. The optimum conditions for uranium leaching were 10% mass fraction of NH4HF2, a liquid-solid ratio of 30:1, a reaction temperature of 30 °C and a reaction time of 120 min, and the leaching efficiency of uranium from the residue was as high as 98.95%. The leaching kinetics of uranium by NH4HF2 were consistent with the mixed controlled model in the shrinking core models, indicating that the surface chemical reaction and mass diffusion dominated both uranium leaching processes. This may provide a viable method for resource recovery and the treatment of uranium purification residues.


Subject(s)
Uranium , Uranium/chemistry , Fluorides/chemistry , Ammonium Compounds/chemistry , Kinetics
17.
Int J Biol Macromol ; 266(Pt 2): 131112, 2024 May.
Article in English | MEDLINE | ID: mdl-38537863

ABSTRACT

In this work, the modified­sodium alginate gel beads were prepared by sol-gel method. Due to the presence of water channels in the sodium alginate gel bead, amidoxime groups and PO43- were exposed to the surface of the adsorbent to the maximum extent, resulting in the excellent adsorption capacity of modified­sodium alginate gel beads. The introduction of amidoxime-modified hydroxyapatite significantly improved the adsorption capacity and the adsorption rate of the gel beads. The adsorption capacity increased from 308.7 to 466.0 mg/g and the adsorption equilibrium time was shortened from 300 min to 120 min. The modified­sodium alginate gel bead possessed the advantages of short adsorption time, high adsorption efficiency and large adsorption capacity, which could be regarded as a potential adsorbent for uranium. Moreover, the uranium removal ability on the modified gel beads was mainly attributed to the Coulomb force between PO43- and uranium and the complexation between uranium and amidoxime groups. In summary, this work would provide a new idea for the modification and application of sodium alginate-based materials.


Subject(s)
Alginates , Durapatite , Gels , Oximes , Uranium , Alginates/chemistry , Uranium/chemistry , Uranium/isolation & purification , Adsorption , Durapatite/chemistry , Oximes/chemistry , Gels/chemistry , Microspheres , Kinetics , Hydrogen-Ion Concentration
18.
Int J Biol Macromol ; 266(Pt 1): 131113, 2024 May.
Article in English | MEDLINE | ID: mdl-38531524

ABSTRACT

In order to prevent uranium pollution and recovery uranium resources, it was necessary to find a highly efficient adsorbent for radioactive wastewater treatment. Herein, U(VI) imprinted polyethyleneimine (PEI) incorporated chitosan/layered hydrotalcite composite foam (IPCL) was synthesized by combining ion-imprinting and freeze-drying techniques. IPCL has a high amino/imino content and an ultralight macroporous structure, making it capable of efficiently adsorbing U(VI) and easy to separate; Especially after ion-imprinting, vacancies matching the size of uranyl ions were formed, significantly improving U(VI) selectivity. The adsorption isotherms and adsorption kinetics were in accordance with the Freundlich model and PSO model respectively, indicating that heterogeneous adsorption of U(VI) by the adsorbents. The adsorption capacity of IPCL-2 for U(VI) reached 278.8. mg/g (under the conditions of optimal pH 5.0, temperature of 298 K, contact time of 2 h, and adsorbent dosage of 0.2 g/L), which is almost double of that for the non-imprinted foam (PCL-2, 138.2 mg/g), indicating that IPCL-2 can intelligently recognize U(VI). The heterogeneous adsorption mechanism of U(VI) by IPCL-2 involves complexation, ion-exchange and isomorphic substitution. The adsorption of U(VI) by IPCL-2 is spontaneous and endothermic. IPCL-2 has excellent adsorption performance for U(VI), and is a promising adsorbent for radioactive pollution control.


Subject(s)
Aluminum Hydroxide , Chitosan , Magnesium Hydroxide , Polyethyleneimine , Uranium , Uranium/chemistry , Polyethyleneimine/chemistry , Chitosan/chemistry , Adsorption , Aluminum Hydroxide/chemistry , Kinetics , Magnesium Hydroxide/chemistry , Porosity , Hydrogen-Ion Concentration , Water Purification/methods , Temperature , Ions/chemistry
19.
Int J Biol Macromol ; 266(Pt 2): 130996, 2024 May.
Article in English | MEDLINE | ID: mdl-38531521

ABSTRACT

Metal-organic frameworks (MOF)-polymer hybrid hydrogel solves the processable forming of MOF powder and energy consumption of uranium extraction. However, the hybrid hydrogel by conventional synthesis methods inevitably lead to MOF agglomeration, poor filler-polymer interfacial compatibility and slowly adsorption. Herein, we designed that ZIF-67 was implanted into the carboxymethyl cellulose/polyacrylamide (CMC/PAM) by network-repairing strategy. The carboxyl and amino groups on the surface of CMC/PAM drive the uniform growth of ZIF-67 inside the CMC/PAM, which form an array of oriented and penetrating microchannels through coordination bonds. Our strategy eliminate the ZIF-67 agglomeration, increase the interfacial compatibility between MOF and polymer. The method also improve the free and fast diffusion of uranium in CMC/PAM/ZIF-67 hydrogel. According to the experimental, these enhancements synergistically enabled the CMC/PAM/ZIF-67 have a maximum adsorption capacity of 952 mg g-1. The adsorption process of CMC/PAM/ZIF-67 fits well with pseudo-second-order model and Langmuir isotherm. Meanwhile, the CMC/PAM/ZIF-67 maintain a high removal rate (87.3 %) and chemical stability even during ten adsorption-desorption cycles. It is worth noting that the adsorption amount of CMC/PAM/ZIF-67 in real seawater is 9.95 mg g-1 after 20 days, which is an ideal candidate adsorbent for uranium extraction from seawater.


Subject(s)
Acrylic Resins , Carboxymethylcellulose Sodium , Metal-Organic Frameworks , Seawater , Uranium , Uranium/chemistry , Uranium/isolation & purification , Adsorption , Acrylic Resins/chemistry , Carboxymethylcellulose Sodium/chemistry , Metal-Organic Frameworks/chemistry , Seawater/chemistry , Hydrogels/chemistry , Kinetics , Water Purification/methods , Water Pollutants, Radioactive/isolation & purification , Water Pollutants, Radioactive/chemistry
20.
Int J Biol Macromol ; 266(Pt 1): 131210, 2024 May.
Article in English | MEDLINE | ID: mdl-38552692

ABSTRACT

The effects of Fe(II) and humic acid on U(VI) immobilization onto oxidized carbon nanofibers (Ox-CNFs, pyrolysis of bacterial cellulose) were investigated by batch, spectroscopic and modeling techniques, with results suggesting that, Ox-CNFs exhibited fast adsorption rate (adsorption equilibrium within 3 h), high adsorption performance (maximum adsorption capacity of 208.4 mg/g), good recyclability (no notable change after five regenerations) in the presence of Fe(II) towards U(VI) from aqueous solutions (e.g., 40 % reduction and 10 % adsorption at pH 8.0), which was attributed to the various oxygen-containing functional groups, excellent chemical stability, large specific surface area and high redox effect. U(VI) adsorption increased with increasing pH from 2.0 to 5.0, then high-level plateau and remarkable decrease were observed at 5.0-6.0 and at pH > 6.0, respectively. According to FT-IR and XPS analysis, a negative correlation between U(VI) reduction and organic in the presence of Fe(II) implied that U(VI) reduction was driven by Fe(II) while inhibited by humic acid. The interaction mechanism of U(VI) on Ox-CNFs was demonstrated to be adsorption and ion exchange at low pH and reduction at high pH according to XPS and surface complexation modeling. These findings filled the knowledge gaps pertaining to the effect of Fe(II) on the transformation and fate of U(VI) in the actual environment. This carbon material with distinctive performance and unique topology offers a potential platform for actual application in environmental remediation.


Subject(s)
Carbon , Cellulose , Humic Substances , Nanofibers , Oxidation-Reduction , Uranium , Humic Substances/analysis , Nanofibers/chemistry , Adsorption , Cellulose/chemistry , Carbon/chemistry , Uranium/chemistry , Pyrolysis , Hydrogen-Ion Concentration , Ferrous Compounds/chemistry , Kinetics , Spectroscopy, Fourier Transform Infrared
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