Functionalized maghemite nanoparticles for enhanced adsorption of uranium from simulated wastewater and magnetic harvesting

被引：33

作者：

Xiao, Yawen ^{[1
]}

Helal, Ahmed S. ^{[1
,2
,3
]}

Mazario, Eva ^{[1
]}

Mayoral, Alvaro ^{[4
]}

Chevillot-Biraud, Alexandre ^{[1
]}

Decorse, Philippe ^{[1
]}

Losno, Remi ^{[5
]}

Maurel, Francois ^{[1
]}

Ammar, Souad ^{[1
]}

Lomas, John S. ^{[1
]}

Hemadi, Miryana ^{[1
]}

机构：

[1] Univ Paris Cite, CNRS, ITODYS, F-75013 Paris, France

[2] MIT, Dept Nucl Sci & Engn, Cambridge, MA 02139 USA

[3] Nucl Mat Author, POB 540, Cairo, Egypt

[4] Univ Zaragoza, Inst Nanociencia Aragon Zaragoza, Aragon, Spain

[5] Univ Paris Cite, Inst Phys Globe Paris, CNRS, F-75005 Paris, France

来源：

ENVIRONMENTAL RESEARCH | 2023年 / 216卷

关键词：

Magnetic nanohybrids; Ligands; Wastewater treatment; pH optimization; DFT calculations; Actinide complexation; Partition coefficient; AQUEOUS-SOLUTION; EFFICIENT; URANYL; THERMODYNAMICS; EXTRACTION; CAPACITY; KINETICS; RECOVERY;

D O I：

10.1016/j.envres.2022.114569

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

Maghemite (gamma-Fe2O3) nanoparticles (MNPs) were functionalized with 3-aminopropyltriethoxysilane (APTES) to give APTES@Fe2O3 (AMNP) which was then reacted with diethylenetriamine-pentaacetic acid (DTPA) to give a nanohybrid DTPA-APTES@Fe2O3 (DAMNP). Nano-isothermal titration calorimetry shows that DTPA complex-ation with uranyl ions in water is exothermic and has a stoichiometry of two DTPA to three uranyl ions. Density functional theory calculations indicate the possibility of several complexes between DTPA and UO22+ with different stoichiometries. Interactions between uranyl ions and DAMNP functional groups are revealed by X-photoelectron and Fourier transform infrared spectroscopies. Spherical aberration-corrected Scanning Trans-mission Electron Microscopy visualizes uranium on the particle surface. Adsorbent performance metrics were evaluated by batch adsorption studies under different conditions of pH, initial uranium concentration and contact time, and the results expressed in terms of equilibrium adsorption capacities (qe) and partition co-efficients (PC). By either criterion, performance increases from MNP to AMNP to DAMNP, with the maximum uptake at pH 5.5 in all cases: MNP, qe = 63 mg g-1, PC = 127 mg g-1 mM-1; AMNP, qe = 165 mg g-1, PC = 584 mg g-1 mM-1; DAMNP, qe = 249 mg g- 1, PC = 2318 mg g-1 mM-1 (at 25 degrees C; initial U concentration 0.63 mM; 5 mg adsorbent in 10 mL of solution; contact time, 3 h). The pH maximum is related to the predominance of mono-and di-cationic uranium species. Uptake by DAMNPs follows a pseudo-first-order or pseudo-second-order kinetic model and fits a variety of adsorption models. The maximum adsorption capacity for DAMNPs is higher than for other functionalized magnetic nanohybrids. This adsorbent can be regenerated and recycled for at least 10 cycles with less than 10% loss in activity, and shows high selectivity. These findings suggest that DAMNP could be a promising adsorbent for the recovery of uranium from nuclear wastewaters.

引用

页数：13