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1.
Chemosphere ; 350: 141184, 2024 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-38215834

RESUMEN

Efficient recognition, separation and recovery of palladium from high-level liquid waste (HLLW) not only helps the safe, green and environmentally friendly disposal of nuclear waste, but also is an essential important supplement to overcome the growing shortage of natural palladium resources. Herein, a novel silica-based functional adsorbent named 2AT-SiAaC was prepared by a two-step method, i.e., grafting of 2-aminothiazole (2AT) via the amidated reaction after in-situ polymerization of acrylic monomers on porous silica. SEM, EDS, TG-DSC, BET and PXRD all proved the successful preparation of 2AT-SiAaC, and it exhibited ultrahigh adsorption selectivity for Pd(II) (Kd (distribution coefficient) ≥ 10,344.2 mL/g, SFPd/M (separation factor) ≥ 613.7), fast adsorption kinetics with short equilibrium time (t ≤ 1 h) and good adsorption capacity (Q ≥ 62.1 mg Pd/g). The dynamic column experiments shows that 2AT-SiAaC achieved efficiently separation of Pd(II) from simulated HLLW, and the enrichment coefficients (C/C0) of Pd(II) was as high as about 14 with the recovery rate nearly 99.9% and basically kept the same performance in three adsorption-desorption column cycle experiments. The adsorption mechanism was analyzed by FT-IR, XPS and DFT calculations, and the ultrahigh selectivity of 2AT-SiAaC was attributed to the preferred affinity of the soft N-donor atoms in 2AT for Pd(II). NO3- ions participated in the adsorption reaction to keep charge balance, and the frontier orbital electron density distribution diagram shows the charge transfer in the process of material preparation and adsorption. To sum up, 2AT-SiAaC adsorbent provided a new insight for precise recognition and efficient separation of Pd(II) from HLLW.


Asunto(s)
Paladio , Tiazoles , Contaminantes Químicos del Agua , Paladio/análisis , Dióxido de Silicio , Espectroscopía Infrarroja por Transformada de Fourier , Adsorción , Cinética
2.
Water Res ; 247: 120819, 2023 Dec 01.
Artículo en Inglés | MEDLINE | ID: mdl-37931357

RESUMEN

To address the imperative need for efficient removal of uranium-containing wastewater and mitigate radioactive contamination risks associated with nuclear energy, the development of materials with high removal efficiency and facile separation is crucial. This study designed and synthesised MnO2@chitosan (CTS) composite aerogel beads by in-situ growing δ-MnO2 on porous CTS aerogel beads. This approach not only mitigates the agglomeration of MnO2 nanospheres but also significantly enhances the porous structure and surface area of MnO2@CTS. These cost-effective and eco-friendly millimeter-scale spherical aerogels exhibited convenient separation properties after adsorption. These characteristics help mitigate the risk of equipment seam blockage and secondary pollution that are often associated with powdered adsorbents. Additionally, MnO2@CTS exhibited remarkable mechanical strength (stress approximately 0.55 MPa at 60 % strain), enabling rapid separation and easy regeneration while maintaining high adsorption performance even after five cycles. Significantly, MnO2@CTS exhibited a maximum adsorption capacity of 410.7 mg/g at pH 6 and 298 K, surpassing reported values for most CTS/MnO2-based adsorbents. The chemisorption process of U(VI) on MnO2@CTS followed the pseudo-second-order kinetic and Dubinin-Radushkevish models. X-ray photoelectron spectroscopy analysis further confirmed the reduction of U(VI) to U(V/IV). These findings highlight the substantial potential of MnO2@CTS aerogel beads for U(VI) removal from aqueous solutions, positioning them as a promising solution for addressing U(VI) contamination in wastewater.


Asunto(s)
Quitosano , Uranio , Aguas Residuales , Uranio/análisis , Quitosano/química , Compuestos de Manganeso , Óxidos , Adsorción , Cinética , Concentración de Iones de Hidrógeno
3.
Materials (Basel) ; 16(3)2023 Jan 27.
Artículo en Inglés | MEDLINE | ID: mdl-36770102

RESUMEN

Sea material is becoming increasingly popular and widely used as an adsorbent in wastewater treatment. Snail shell, a low-cost and natural animal waste material, has been shown to have a high calcium content (>99%) and a large potential surface area for the development of sustainable adsorbents. This paper presents a novel synthesis of methods for using snail shell absorbent materials in the treatment of wastewater containing heavy metals, textile dyes, and other organic substances. Modified biochar made from snail shells has gained popularity in recent years due to its numerous benefits. This paper discusses and analyzes modification methods, including impregnating with supplements, combining other adsorbents, synthesis of hydroxyapatite, co-precipitation, and the sol-gel method. The analysis of factors influencing adsorption efficiency revealed that pH, contact time, temperature, initial concentration, and adsorbent dose all have a significant impact on the adsorption process. Future research directions are also discussed in this paper as a result of presenting challenges for current snail adsorbents.

4.
Chemosphere ; 308(Pt 3): 136546, 2022 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-36152829

RESUMEN

As one of the most frequently used nuclides for nuclear fuel and toxic heavy metal in polluted solutions, the removal and recovery of U(VI) from wastewater is significant both for nuclear energy and human health. Herein, the novel hierarchical Mg-Al bimetallic oxides (Mg/Al-BOs) were successfully synthesized by a facile hydrothermal-lyophilization-calcination method for enhanced removal of uranium (U(VI)) from wastewater. The as-synthesized Mg/Al-BOs adsorbents were characterized by a variety of techniques including SEM-EDS, XRD, high temperature in-situ XRD, TG-DSC, N2 adsorption-desorption isotherm and XPS. Batch experiments including the effects of pH, hydration species, interfering ions on U(VI) removal, adsorption kinetics, isotherms and recyclability were systematically studied. Results showed that calcined Mg/Al-BO-24 inherited the hierarchical structure from its hydrotalcite-like precursor and grew the bimetallic oxides of Al2O3/MgO into a 3D rod-like and mesoporous network with the large BET surface area (472.4 m2∙g-1), which presented abundant binding sites on the surface and contributed to preventing the aggregation of Al2O3/MgO nanoparticles, allowing the fast uptake of U(VI) for equilibrium within 180 min and the significant increase of maximum adsorption capacity to 411.5 mg∙g-1. The uptake kinetics and isotherms of U(VI) removal could be well represented by the pseudo-second-order and Langmuir models, respectively. Further, it was demonstrated that U(VI) removal by Mg/Al-BO-24 was less influenced by coexisting cations and the regeneration cycles, indicating the excellent selectivity and reusability for U(VI) by the as-prepared composites. Based on the XPS analysis results, the mechanisms for U(VI) sorption onto the Mg/Al-BO-24 were mainly ascribed to the synergistic surface complexation and electrostatic interaction. These results suggested that Mg/Al-BO-24 prepared by the method reported here was available for developing other multiple metal oxides and would be a promising material for the effective treatment of wastewater with U(VI)-contamination.


Asunto(s)
Uranio , Adsorción , Cationes , Humanos , Concentración de Iones de Hidrógeno , Cinética , Óxido de Magnesio , Óxidos/química , Uranio/análisis , Aguas Residuales
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