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1.
J Hazard Mater ; 467: 133741, 2024 Apr 05.
Artículo en Inglés | MEDLINE | ID: mdl-38341887

RESUMEN

Radioactive strontium (90Sr) is considered as one of the most dangerous radionuclides due to its high biochemical toxicity. For the efficient and selective separation of Sr from acidic environments, a novel functional adsorbent CEPA@SBA-15-APTES was prepared in this work through the phosphorylation of amino-modified mesoporous silica with organic content of approximately 20 wt%. CEPA@SBA-15-APTES was characterized by TEM, SEM, EDS, TG-DSC, BET, FTIR, and XPS techniques, revealing its characteristics of an ordered hexagonal lattice-like structure and rich functional groups. The experimental results demonstrated that the adsorbent exhibited good adsorption capacity for Sr over a wide acidity range (i.e., from 10-10 M to 4 M HNO3). The adsorption equilibriums of Sr by CEPA@SBA-15-APTES in 10-6 M and 3 M HNO3 solutions were reached within 30 and 5 min, respectively, and the adsorption capacities at 318 K were 112.6 and 71.8 mg/g, respectively. Furthermore, by combining the experimental and characterization results, we found that the adsorption mechanism consisted of ion exchange between Sr(II) and H+ (in P-OH) in the 10-6 M HNO3 solution and coordination between the Sr(II) and oxygen-containing (CO and P = O) functional groups in the 3 M HNO3 solution.

2.
Small ; : e2311916, 2024 Feb 12.
Artículo en Inglés | MEDLINE | ID: mdl-38344887

RESUMEN

Surface defects on photocatalysts could promote carrier separation and generate unsaturated sites for chemisorption and reactant activation. Nevertheless, the inactivation of oxygen vacancies (OVs) would deteriorate catalytic activity and limit the durability of defective materials. Herein, bagasse-derived carbon quantum dots (CQDs) are loaded on the Sn-doped Bi2 O2 CO3 (BOC) via hydrothermal procedure to create Bi─O─C chemical bonding at the interface, which not only provides efficient atomic-level interfacial electron channels for accelerating carriers transfer, but also enhances durability. The optimized Sn-BOC/CQDs-2 achieves the highest photocatalytic removal efficiencies for levofloxacin (LEV) (88.7%) and Cr (VI) (99.3%). The elimination efficiency for LEV and Cr (VI) from the Sn-BOC/CQDs-2 is maintained at 55.1% and 77.0% while the Sn-BOC is completely deactivated after four cycle tests. Furthermore, the key role of CQDs in stabilization of OVs is to replace OVs as the active center of H2 O and O2 adsorption and activation, thereby preventing reactant molecules from occupying OVs. Based on theoretical calculations of the Fukui index and intermediates identification, three possible degradation pathways of LEV are inferred. This work provides new insight into improving the stability of defective photocatalysts.

3.
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
4.
J Colloid Interface Sci ; 629(Pt B): 97-110, 2023 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-36152584

RESUMEN

The synergistic effect between transition metal active centers and the generation of multiple removal pathways has a significant impact on the catalytic activation efficiency of peroxymonosulfate. In this work, a kind of composite catalyst was prepared by growing VCo-metal-organic frameworks (VCo-MOF) in-situ on the surface of Ti3C2Tx by a solvothermal method. The morphology and structure are characterized by Transmission Electron Microscope (TEM), Energy Dispersion Spectrum (EDS), Atomic Force Microscope (AFM), etc. Response surface methodology was used to optimize the experimental conditions. Only 5 mg catalyst can be used to effectively activate PMS and remove 96.14 % ciprofloxacin (CIP, 20 mg/L) within 30 min. The removal effect of catalyst on CIP in different actual water environment was explored. In addition, the fluorescence spectrum test also verified the effective removal of ciprofloxacin. V-Co-Ti ternary system provides a wealth of active sites for CIP removal. Cyclic voltammetry (CV) and lear sweep voltammetry (LSV) tests showed the existence of the electron transfer pathway. The results of density functional theory (DFT) calculation show that VCo-MOF@Ti3C2Tx has excellent adsorption and activation ability for PMS. At the same time, the hydrophilicity of the catalyst makes PMS more inclined to react with water molecules, which promotes the formation of a unique superoxide radical path.

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