RESUMO
Based on the goal of "carbon neutralization and carbon peaking", it is still challenging to develop a high adsorption performance and environmentally friendly material for uranium extraction. We proposed a new idea of "Three-Dimensional Environmental-Friendly". A series of amino acid bis-substituted chitosan aerogels (C-1, C-2, C-3, C-4 and C-5) were prepared by ice template method and selective substitution reaction in water environment. Among them, C-3 adsorbent has the antibacterial properties of gram-positive bacteria, gram-negative bacteria and marine bacteria, which is more suitable for uranium adsorption in complex environments. Also, C-3 adsorbent solves the shortcomings of poor adsorption property and easy to cause secondary pollution during modification of traditional chitosan materials. The selectivity and adsorption capacity of uranium are further improved by the unique functional groups of serine residues. At pH = 7, the maximum adsorption capacity reaches 606.32 mg/g. In addition, C-3 adsorbent have excellent selectivity and stability. The synergistic effect of coordination, electrostatic interaction and intraparticle diffusion between C-3 adsorbent and uranium may be the key to its high adsorption performance. The high performance of chitosan adsorbent provides a new idea for the design and application of green and efficient uranium adsorption materials.
Assuntos
Aminoácidos , Antibacterianos , Quitosana , Urânio , Quitosana/química , Urânio/química , Adsorção , Antibacterianos/farmacologia , Antibacterianos/química , Aminoácidos/química , Géis/química , Concentração de Íons de HidrogênioRESUMO
Marine biofouling directly affects the performance and efficiency of uranium (U(VI)) extraction from seawater. Compared to traditional chemical methods, natural plant extracts are generally biodegradable and nontoxic, making them an environmentally friendly alternative to synthetic chemicals in solving the marine biofouling problem. The effectiveness of natural antibacterial plants (i.e., pine needle, peppermint, Acorus gramineus Soland, Cacumen platycladi, and wormwood) in solving the marine biofouling problem was evaluated in this work. Experimental results showed that natural antibacterial plants could kill Vibrio alginolyticus in solution and effectively solve the marine biofouling problem of U(VI) extraction. To improve the adsorption capacity of natural plants for U(VI) in seawater, poly(vinylphosphonic acid) (PVPA) was modified on natural antibacterial plant surfaces by irradiation grafting technology. PVPA and natural antibacterial plants work as active sites and base materials for the U(VI) extraction material, respectively. The recovery performance of PVPA/pine needle for U(VI) was preliminarily studied. Results show that the adsorption of U(VI) on PVPA/pine needle follows pseudo-second-order and Langmuir models, and the maximum adsorption capacity is 111 mg/g at 298 K and pH 8.2.
Assuntos
Antibacterianos , Água do Mar , Urânio , Urânio/química , Urânio/isolamento & purificação , Antibacterianos/farmacologia , Antibacterianos/química , Antibacterianos/isolamento & purificação , Água do Mar/microbiologia , Teste de Materiais , Adsorção , Materiais Biocompatíveis/química , Materiais Biocompatíveis/farmacologia , Materiais Biocompatíveis/isolamento & purificação , Tamanho da Partícula , Extratos Vegetais/química , Extratos Vegetais/farmacologia , Extratos Vegetais/isolamento & purificação , Poluentes Radioativos da Água/isolamento & purificação , Poluentes Radioativos da Água/químicaRESUMO
This study proposes the use of diglycolamic acid-functionalized graphitic carbon nitride (HDGA-gCN) as an adsorbent for uranium removal. Our experiments showed that at pH 6.0, HDGA-gCN had a high adsorption capacity of 263.2 mg g-1 and achieved equilibrium in 30 min. The adsorption isotherm was well-fitted by the Langmuir model, and the adsorption kinetics followed a pseudo-second-order equation. U(VI) adsorption on HDGA-gCN is due to electrostatic interactions between the amine, diglycolamic acid, and uranium species. The thermodynamic parameters indicate that adsorption is spontaneous and exothermic. The loaded U(VI) can be desorbed using 0.1 M Na2CO3, and HDGA-gCN exhibited an exceptional adsorption percentage for U(VI) compared to other coexisting ions. HDGA-gCN had faster kinetics, adsorption capacity, and reusability, making it suitable for U(VI) remediation.
Assuntos
Grafite , Termodinâmica , Urânio , Urânio/química , Adsorção , Cinética , Grafite/química , Compostos de Nitrogênio/químicaRESUMO
The combined chemotoxicity and radiotoxicity associated with uranium, utilized in nuclear industry and military applications, poses significant threats to human health. Among uranium pollutants, uranyl is particularly concerning due to its high absorptivity and potent nephrotoxicity in its + 6 valence state. Here, we have serendipitously found Na2SeO3 facilitates the conversion of U(VI) to U(IV) precipitates. A novel approach involving nano-chitosan loaded internally with melatonin and externally modified with selenite (NPs Cs-Se/MEL) was introduced. This modification not only enhances the conversion of U(VI) to U(IV) but also preserves the spherical nanostructure and specific surface area, leading to increased adsorption of U(VI) compared to unmodified samples. Selenite modification improves lysosomal delivery in HEK-293 T cells and kidney distribution of the nanoparticles. Furthermore, NPs Cs-Se/MEL demonstrated a heightened uranium concentration in urine and exhibited remarkable efficiency in uranium removal, resulting in a reduction of uranium deposition in serum, kidneys, and femurs by up to 52.02 %, 46.79 %, and 71.04 %, respectively. Importantly, NPs Cs-Se/MEL can be excreted directly from the kidneys into urine when carrying uranium. The results presented a novel mechanism for uranium adsorption, making selenium-containing nano-materials attractive for uranium sequestration and detoxification.
Assuntos
Quitosana , Melatonina , Nanopartículas , Ácido Selenioso , Urânio , Humanos , Urânio/química , Células HEK293 , Melatonina/administração & dosagem , Melatonina/química , Melatonina/farmacocinética , Quitosana/química , Nanopartículas/química , Ácido Selenioso/química , Animais , Rim/metabolismo , Rim/efeitos dos fármacos , Adsorção , Masculino , Distribuição TecidualRESUMO
In this work, chemical modification of the chitosan with ethyl acetoacetate was performed through a base-catalyzed reaction in which epichlorohydrin facilitated the insertion as well as nucleophilic substitution reaction to graft the 1,3-dioxo moiety across the linear chains of the base biopolymer to establish specificity and selectivity for U(VI) removal. The modified chitosan (EAA-CS) was intercalated into phosphate rich alginate matrix (PASA). Later on, the WO3-doped composites with different WO3 to PASA mass ratio were prepared and characterized using FTIR, XPS, SEM-EDS, XRD, and elemental mapping analysis. WO3 significantly contributed to chemically stable inorganic-organic composites with improved porous texture. Among the prepared composites, MCPS-3 microspherical beads, having mass ratio of 30.0 % w/w, exhibited excellent sorption capacity for U(VI) at an optimal pH 4.5. The successful U(VI) sorption was validated by the existence of two U4f peaks at 392.25 and 381.36 eV due to U4f5/2 and U4f7/2 sub-peaks with an intensity ratio of 3:4, respectively. Batch mode sorption kinetics followed pseudo-second-order rate equation (R2 ≈ 0.99, qe,th ≈ 116.88 mg/g, k2 = 0.86 × 10-4 g/mg.min-1) and equilibrium sorption data aligns with Langmuir (R2 = 0.99, qm = 343.85 mg/g at 310 K and pH = 4.5, KL = 2.00 × 10-2 L/mg) and Temkin models (R2 ≈ 0.99). Thermodynamic parameters ΔHo (30.51 kJ/mol), ΔSo (0.19 kJ/mol.K) and ΔGo (-25.64, -26.89, and - 27.91 kJ/mol) at 298, 305, and 310 K, respectively, suggested that the uptake process is feasible, endothermic and spontaneous. Based on these findings, it is reasonable to conclude that MCPS-3 could be a better hydrogel-based biomaterial for appreciable uranium recovery.
Assuntos
Alginatos , Quitosana , Óxidos , Ácido Fítico , Tungstênio , Urânio , Quitosana/química , Alginatos/química , Adsorção , Tungstênio/química , Óxidos/química , Ácido Fítico/química , Urânio/química , Cinética , Concentração de Íons de Hidrogênio , Purificação da Água/métodosRESUMO
Calculation of thermodynamic parameters of adsorption such as Gibbs free energy ΔG°ads from experimentally determined adsorption data can be helpful for elucidation of sorption mechanisms. This approach includes the transformation of adsorption coefficients Kd or KL into dimensionless standard adsorption constants Kads [-]. The present comment reveals recently published misleading approaches and offers thermodynamically sound alternatives.
Assuntos
Termodinâmica , Urânio , Adsorção , Urânio/química , Carvão Vegetal/química , Polímeros/químicaRESUMO
The presence of carbonates or humic substances (HS) will significantly affect the species and chemical behavior of U(VI) in solution, but lacking systematic exploration of the coupling effect of carbonates and HS under near real environmental conditions at present. Herein, the sorption behavior of U(VI) on illite was systematically studied in the co-existence of carbonates and HS including both humic acid (HA) and fulvic acid (FA) by batch technique. The distribution coefficients (Kd) increased as function of time and temperature but decreased with increasing concentrations of initial U(VI), Ca2+, and Mg2+, as well as ion strength. At pH 2.0-10.5, the Kd values first increased rapidly and then decreased visibly, with its maximum value appearing at pH 5.0, owning to the changes in the interaction between illite and the dominant species of U(VI) from electrostatic attraction to electrostatic repulsion. The sorption was a heterogeneous, spontaneous, and endothermic chemical process, which could be well described by pseudo-second-order kinetic and Flory-Huggins isotherm models. When carbonates and HA/FA coexisted, the Kd values always increased first and then decreased as a function of pH, with the only difference for HA and FA being the key pH (pHkey) at which the promoting and inhibiting effects on the sorption of U(VI) onto illite undergo a transition. The carbonates and HS have a synergistic inhibitory effect on the U(VI) sorption onto illite at pH 7.8. FTIR and XPS spectra demonstrated that the hydroxyl groups on the illite surface and in the HS were involved in U(VI) sorption on illite in the presence of carbonates. These results provide valuable data for a deeper understanding of U(VI) migration in geological media.
Assuntos
Carbonatos , Substâncias Húmicas , Minerais , Urânio , Adsorção , Carbonatos/química , Urânio/química , Minerais/química , Modelos Químicos , Benzopiranos/química , CinéticaRESUMO
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.
Assuntos
Água Subterrânea , Osmose , Urânio , Poluentes Radioativos da Água , Purificação da Água , Urânio/química , Água Subterrânea/química , Purificação da Água/métodos , Concentração de Íons de Hidrogênio , Adsorção , Poluentes Radioativos da Água/química , Poluentes Radioativos da Água/análise , Íons/químicaRESUMO
Polyethylene terephthalate (PET) plastics find widespread use in various aspects of our daily lives but often end up in the environment as (micro)plastic waste. In this study, the adsorption efficiency of PET microplastics for U-232 has been investigated prior and after surface alteration (e.g. oxidation (PET-ox), MnO2-coating (PET/MnO2) and biofilm-formation (PET/Biofilm)) in the laboratory (at pH 4, 7 and 9) and seawater samples under ambient conditions and as a function of temperature. The results revealed a significant increase in the adsorption efficiency upon surface alteration, particularly after biofilm development on the MP's surface. Specifically, the Kd values evaluated for the adsorption of U-232 by PET, PET-ox, PET/MnO2 and PET/Biofilm are 12, 27, 73 and 363, respectively, at pH 7 and under ambient conditions. The significantly higher adsorption efficiency of the altered and particularly biofilm-coated PET, emphasizes the significance of surface alteration, which may occur under environmental conditions. In addition, according to the thermodynamic investigations the adsorption of U-232 by PET-MPs (both non-treated and modified), the adsorption is an endothermic and entropy-driven reaction. A similar behavior has been also observed using seawater solutions and assumes that surface alteration is expected to enhance the radionuclide, stability, mobility and bioavailability in environmental water systems.
Assuntos
Biofilmes , Microplásticos , Polietilenotereftalatos , Polietilenotereftalatos/química , Adsorção , Microplásticos/química , Água do Mar/química , Urânio/química , Termodinâmica , Concentração de Íons de Hidrogênio , Propriedades de Superfície , Temperatura , Óxidos/química , Poluentes Radioativos da Água/química , OxirreduçãoRESUMO
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.
Assuntos
Água Subterrânea , Mineração , Urânio , Urânio/química , China , Água Subterrânea/química , Permeabilidade , Movimentos da Água , Poluentes Radioativos da Água/análise , Poluentes Radioativos da Água/química , PorosidadeRESUMO
The reaction between the lixiviant and the minerals in the aquifer of In-situ uranium leaching (ISL) will result mineral dissolution and precipitation. ISL will cause changes in the chemical composition of groundwater and the porosity and permeability of aquifer, as well as groundwater pollution. Previous studies lack three-dimension numerical simulation that includes a variety of minerals and considers changes in porosity and permeability properties simultaneously. To solve these problems, a three-dimensional reactive transport model (RTM) which considered minerals, main water components and changes in porosity and permeability properties in Bayanwula mine has been established. The results revealed that: (1) Uranium elements were mainly distributed inside the mining area and had a weak trend of migration to the outside. The strong acidity liquid is mainly in the mining area, and the acidity liquid dissolved the minerals during migrating to the outside of the mining area. The concentration front of major metal cations such as K+, Na+, Ca2+ and Mg2+ is about 150m away from the boundary. (2) The main dissolved minerals include feldspar, pyrite, calcite, sodium montmorillonite and calcium montmorillonite. Calcite is the most soluble mineral and one of the sources of gypsum precipitation. Other minerals will dissolve significantly after calcite is dissolved. (3) ISL will cause changes in porosity and permeability of the mining area. Mineral dissolution raises porosity and permeability near the injection well. Mineral precipitation reduced porosity and permeability near the pumping well, which can plugging the pore throat and affect recovery efficiency negatively.
Assuntos
Água Subterrânea , Minerais , Mineração , Urânio , Urânio/análise , Urânio/química , Água Subterrânea/química , Água Subterrânea/análise , China , Minerais/análise , Minerais/química , Poluentes Radioativos da Água/análise , Poluentes Radioativos da Água/química , PorosidadeRESUMO
The development and exploration of uranium decorporation agents with straightforward synthesis, high removal ability, and low toxicity are crucial guarantees for the safety of workers in the nuclear industry and the public. Herein, we report the use of traditional Chinese medicine licorice for uranium decorporation. Licorice has good adsorption performance and excellent selectivity for uranium in the simulated human environment. Glycyrrhizic acid (GL) has a high affinity for uranium (p(UO2) = 13.67) and will complex with uranium at the carbonyl site. Both licorice and GL exhibit lower cytotoxicity compared to the commercial clinical decorporation agent diethylenetriamine pentaacetate sodium salts (CaNa3-DTPA). Notably, at the cellular level, the uranium removal efficiency of GL is eight times higher than that of CaNa3-DTPA. Administration of GL by prophylactic intraperitoneal injection demonstrates that its uranium removal efficiency from kidneys and bones is 55.2 and 23.9%, while CaNa3-DTPA shows an insignificant effect. The density functional theory calculation of the bonding energy between GL and uranium demonstrates that GL exhibits a higher binding affinity (-2.01 vs -1.15 eV) to uranium compared to DTPA. These findings support the potential of licorice and its active ingredient, GL, as promising candidates for uranium decorporation agents.
Assuntos
Produtos Biológicos , Glycyrrhiza , Ácido Glicirrízico , Urânio , Glycyrrhiza/química , Urânio/química , Urânio/isolamento & purificação , Humanos , Ácido Glicirrízico/química , Ácido Glicirrízico/farmacologia , Ácido Glicirrízico/isolamento & purificação , Produtos Biológicos/química , Produtos Biológicos/farmacologia , Produtos Biológicos/isolamento & purificação , Produtos Biológicos/síntese química , Animais , Teoria da Densidade Funcional , Camundongos , Sobrevivência Celular/efeitos dos fármacosRESUMO
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 gâ»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.
Assuntos
Carvão Vegetal , Hidróxidos , Magnésio , Fosfatos , Urânio , Carvão Vegetal/química , Adsorção , Urânio/química , Fosfatos/química , Magnésio/química , Hidróxidos/química , Alumínio/química , Cinética , Poluentes Químicos da Água/química , Poluentes Químicos da Água/análise , Hidróxido de Alumínio/químicaRESUMO
Uranium recovery from wastewater or seawater is important for both pollution control and uranium supply. Due to the complexity of the water body, it requires that the adsorbent should not only be highly efficient for selective adsorption but also have good antimicrobial properties. In this study, an antimicrobial thermosensitive hydrogel (UITAC) for uranium adsorption was prepared by one-step ion-imprinted polymerization using chitosan as a substrate and allyl trimethylammonium chloride as the antimicrobial modifier. UITAC showed excellent antibacterial rate against Escherichia coli and Staphylococcus aureus, being 98.8 % and 89.1 %, respectively. Endothermic and exothermic peaks respectively showed up at 36.3-38.5 °C and 30.5-34.1 °C in the DSC curves. UITAC quickly achieved its adsorption equilibrium in 30.0 min at 50 °C, pH 5.0 in the 0.8 mg/mL UO22+ solution, with an adsorption capacity of 81.2 mg/g. The adsorption capacity could remain at 80 % after 5 cycles of repeated use. UITAC showed better adsorption selectivity to UO22+ than vanadium and other metal ions, with selectivity coefficients α(UO22+/Mn+) being 1.4-10.3. The pseudo-second-order kinetics and Langmuir adsorption model had a better fit for UO22+ adsorption by UITAC. The adsorption was a spontaneous process. The Gibbs Free Energy change, enthalpy change, and entropy change at 323.2 K were - 16.0 kJ/mol, 64.3 kJ/mol, and 248.4 J/mol·K, respectively. UITAC showed high potential in practical application environment.
Assuntos
Quitosana , Hidrogéis , Compostos de Amônio Quaternário , Compostos de Urânio , Quitosana/química , Adsorção , Hidrogéis/química , Compostos de Amônio Quaternário/química , Compostos de Urânio/química , Staphylococcus aureus/efeitos dos fármacos , Escherichia coli/efeitos dos fármacos , Anti-Infecciosos/química , Anti-Infecciosos/farmacologia , Urânio/química , Temperatura , Cinética , Concentração de Íons de Hidrogênio , Antibacterianos/química , Antibacterianos/farmacologiaRESUMO
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.
Assuntos
Fibra de Algodão , Oximas , Urânio , Urânio/química , Adsorção , Oximas/química , Esgotos/química , Esgotos/microbiologia , Cinética , Antibacterianos/farmacologia , Antibacterianos/química , Purificação da Água/métodosRESUMO
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.
Assuntos
Ferro , Fosfatos , Ferro/química , Fosfatos/química , Adsorção , Urânio/químicaRESUMO
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.
Assuntos
Glucanos , Oximas , Urânio , Glucanos/química , Oximas/química , Urânio/química , Adsorção , Química Click/métodos , Cinética , Poluentes Químicos da Água/química , Poluentes Químicos da Água/isolamento & purificação , Purificação da Água/métodos , Concentração de Íons de Hidrogênio , Íons/químicaRESUMO
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.
Assuntos
Carvão Vegetal , Urânio , Águas Residuárias , Carvão Vegetal/química , Urânio/química , Águas Residuárias/química , Resíduos Radioativos/análise , Poluentes Radioativos da Água , Fosfatos de Cálcio/químicaRESUMO
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.
Assuntos
Bacillaceae , Carbonato de Cálcio , Matriz Extracelular de Substâncias Poliméricas , Metais Pesados , Tório , Urânio , Urânio/química , Urânio/metabolismo , Carbonato de Cálcio/química , Tório/química , Matriz Extracelular de Substâncias Poliméricas/metabolismo , Matriz Extracelular de Substâncias Poliméricas/química , Bacillaceae/metabolismo , Metais Terras Raras/química , Adsorção , Precipitação QuímicaRESUMO
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.