JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Qihang Sun,Baoyu Li,Jiaxin Hu,Hongquan Fu,Juan Zhang,Jinming Chang,Hejun Gao,Yunwen Liao
U(VI) in nuclear wastewater threatens human health and the environment due to its high toxicity and mobility. Photocatalysis is seen as a promising, simple, low-cost, and sustainable method for wastewater treatment, but existing photocatalysts face challenges like complex preparation and severe electron-hole recombination. In this work, ellipsoidal Se-linked ZnSe/ZnO was in situ constructed using a simple one-pot hydrothermal method, with non-metallic selenium serving as the carrier. In 30 minutes, the removal rate of U(VI) can reach 90.2 % in 100 mg/L U(VI) solution. The reaction kinetics of the optimal Se/ZnSe/ZnO ratio reached 0.14939 min −1 , which is nearly 10 times that of pure ZnO. Photocatalytic analysis revealed that introducing Se as the medium for electron transport in the composite material can effectively reduce electron-hole recombination, thereby enhancing photocatalytic efficiency. The results of this study offer a simple and efficient new method for photocatalytic reduction of U(VI) and provide an effective strategy for establishing a conductive medium in the heterojunction using a one-pot hydrothermal method.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Liya Zhang,Xiangrong Wang,Qina Yu,Can Cheng,Aixin Song,Jingcheng Hao
The adsorption of uranium (VI) from wastewater is vital for environment treatment and sustainable growth of the nuclear energy industry. The porous adsorbents with excellent adsorption capacity can be efficiently fabricated by the template from surfactant stabilized foams, but the template is rather susceptible and easily destabilized, resulting in the unsatisfactory performance for target materials. In this work, we proposed a cooperative method using Schiff base reaction combining with surfactant foaming for constructing stable porous templates. A surfactant, cocamidopropyl betaine (CAB), was applied to stabilize foams containing chitosan (CS), glutaraldehyde (GA), acrylamide (AAm) and acrylic acid (AA). The Schiff base reaction between CS and GA endowed the foams with superior stability due to the formation of 3D network in the fluid films. A secondary network generated by polymerizing acrylamide (AAm) and acrylic acid (AA) further reinforced the structure, yielding a highly porous adsorbent (89.5% porosity). The adsorbent, CGAA@NTs, achieved a high U(VI) uptake capacity of 826 mg·g -1 under light irradiation thanks to the incorporation of carboxylated carbon nanotubes (CCNTs), which conferred the adsorbent with excellent photothermal performance, creating a local heat environment to facilitate the U(VI) uptake under light irradiation. Meanwhile, in the complex environment of wastewater, the abundant functional groups (e.g., −NH 2 and −COOH) enabled rich interactions with U(VI) via electrostatic effect and metal-coordination, opening an avenue for exploiting highly porous adsorbents of U(VI) using stable foams as templates.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2025
·
IF 3.5
Yu Liu,Changting Chen,Jianqiang Luo,Shujuan Liu,Jianguo Ma
Photoelectrocatalytic (PEC) reduction of soluble U(VI) to insoluble U(IV) represents a highly promising strategy for uranium removal. The design of photoelectrode materials with superior photoelectrochemical performance is crucial for enhancing PEC efficiency. In this study, an MXene-supported Co-NC (Co-NC/MXene) photoelectrode was successfully fabricated through electrostatic self-assembly. Compared to individual electrocatalytic (EC) and photocatalytic (PC) systems, the PEC system achieved an optimal U(VI) removal efficiency of 99.1 % with a rate constant of 0.116 min −1 , demonstrating reaction rates 13.4 times and 29.3 times higher than those of EC and PC systems, respectively. The Co-NC/MXene electrode exhibited exceptional adsorption capacity (3993.54 mg g −1 for 500 ppm) and maintained over 80 % removal efficiency after six consecutive cycles, highlighting its outstanding stability. This work provides novel insights into the application of MOF-derived/MXene materials for highly efficient U(VI) removal from aqueous solutions.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Long Geng,Yun Zhou,Yaowen Zhang,Lipeng Han,Yuankun Liu,Kesheng Hu,Yun Zhou,Fei Wu,Tonghuan Liu,Junqiang Yang,Keliang Shi,Xiaolin Hou
Uranium-235 enrichment generates highly alkaline effluents rich in fluoride and uranyl species, which pose significant challenges to conventional treatment technologies. Herein, we report a polyamine-amide adsorbent (MF-PAA) obtained by densely grafting amide units and multi-level amine groups onto a fluoride-inert, macroporous MA-DVB scaffold, creating a surface rich in O, N multidentate binding sites. MF-PAA exhibits an exceptional adsorption capacity 1.43 × 10 3 mg·g −1 for U(VI), and retains 625 mg·g −1 capacity even under 8000 ppm F − . Even in 0.50 mol·L −1 competing anions, the material removes 80–90% of U(VI) and achieves a distribution coefficient of 5.0 × 10 5 mL·g −1 under cationic competition conditions, confirming outstanding anion tolerance and selectivity. Mechanistic studies combining spectroscopy and density functional theory (DFT) calculations reveal the most stable uranyl-MF-PAA complex (ΔG = −115.66 kJ/mol), in which uranyl coordinates with O and N atoms of two amide groups in adjacent chains, forming six coordination bonds with mixed ionic-covalent character dominated by U 5f/6d, N 2p, and O 2s/2p orbital interactions. In column operation with a continuous 8000 ppm F − influent, MF-PAA recovered 94% of U(VI), and its capacity maintained after 15 days of high-fluoride exposure, confirming its long-term engineering viability. These results underscore MF-PAA as a robust, renewable, and high-capacity adsorbent with strong potential for uranium recovery from fluoride-rich wastewater.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Lei-Tao Sha,Qiang Wu,Yi-Fan Zhang,Wei-Jia Wang,Fei Wu,Qing-Gang Huang,Ze-Yi Yan
The hydrophobic deep eutectic solvents (HDES) with low viscosity, density and environmental friendliness have been prepared and characterized based on trioctylphosphine oxide (TOPO) and N,N -dihexyl succinamic acid (DHSCA), which were used as both extractant and organic phase for highly efficient removal of radioactive elements of U(VI) and Th(IV) from rare earth (RE) leaching solution. The extraction efficiency of U(VI) and Th(IV) exceeded 99 % by a single stage extraction. Benefiting from the blocking effect of hydrogen bonding on P = O and the good affinity of DHSCA and TOPO for actinides, the present HDES exhibited the excellent extraction selectivity for U(VI) and Th(IV) over Fe(III), Al(III), Mg(II), Ca(II) and RE(III). Even after seven extraction-stripping cycles, the prepared HDES could still effectively remove radioactive U(VI) and Th(IV) from RE leaching solution. The co-extracted U(VI) and Th(IV) was further separated and enriched by two successive stripping steps. Using the slope analysis, 31 P NMR and FT-IR spectra, the stoichiometry of extracted species and the extraction mechanism of HDES to Th(IV) and U(VI) were evaluated. Due to the superior extraction efficiency, excellent environmental compatibility and sustainability, the present approach offers a practical alternative for removal of radioactive elements from rare earth minerals.
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DESALINATION
·
2025
·
IF 9.8
Xiaoying Lin,Bingqing Huang,Yifan Liu,Yuancai Lv,Chunxiang Lin,Jianhui Huang,Minghua Liu,Xiaoxia Ye,Jie Chen
The development of adsorbents capable of simultaneously achieving high uranium(VI) adsorption capacity, rapid kinetics, and exceptional selectivity remains a critical challenge for sustainable uranium(VI) extraction from seawater, essential for nuclear energy sustainability. Herein, we report the synthesis of a novel ellagic acid immobilized conjugated micro-mesoporous poly(aniline)s (CMP-E) via a Buchwald-Hartwig coupling strategy incorporating ellagic acid prefunctionalization. This synergistic combination of molecular confinement and pore engineering maximizes the density of accessible adsorption sites, overcoming the long-standing trade-off between adsorption site uniformity and surface coverage in conventional adsorbents. The resulting CMP-E showed exceptional uranium(VI) extraction performance, achieving a record adsorption capacity of 515 ± 14 mg g −1 , and the initial adsorption kinetics ( h ) reached 6.5 ± 0.3 mg g −1 min −1 , both exceeding pristine CMP by over 1.5 times. Notably, CMP-E demonstrated outstanding selectivity for uranium(VI), with a selectivity coefficient over 6.8 for uranium(VI)/other ions in the presence of various co-existing ions. This enhanced performance was attributed to the stable negative surface charge of CMP-E across a wide pH range, which promoted efficient electrostatic enrichment of uranium(VI) species. The subsequent coordination of uranium(VI) with lone pair electrons from nitrogen atoms (-NH- and = N-) in the poly(aniline) skeleton and oxygen atoms (-OH and C O) in the ellagic acid moiety further enhanced the uranium(VI) capture. Dynamic adsorption tests in real seawater demonstrated promising performance, achieving >86.3 ± 0.9 % uranium(VI) recovery with negligible capacity loss. Furthermore, a 7-day marine field test conducted in Pingtan revealed an adsorption capacity of 2.32 ± 0.02 mg g −1 under real marine conditions. These results suggested that CMP-E held significant potential as a material for the efficient extraction and recovery of uranium(VI) from seawater.
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Journal of Cleaner Production
·
2021
·
IF 9.297
Hao Tang,Shu Zhang,Hongwei Pang,Jiaqi Wang,Xiangxue Wang,Gang Song,Shujun Yu
Radioactive pollutants have always been the top priority in wastewater, and searching a green and efficient treatment technology remains a significant challenge. In this study, a novel melamine sponge supported sulfurized nanoscale zero-valent iron (MS@S-NZVI) material with high dispersion was firstly designed to effectively capture U(VI) from water environment. The target material could retain its original structure in water due to the excellent mechanical strength of MS, which greatly inhibited the aggregation of S-NZVI. A series of characterization techniques, such as SEM, XRD , FTIR, TGA and XPS , had proved the effective synthesis and excellent structural properties of the MS@S-NZVI. The faster reaction equilibrium (<1 h) and higher maximum adsorption capacity (180 mg/g at pH = 5 and 298 K) exposed the perfect performance of target material in the elimination of U(VI). In addition, further researches in different water systems exhibited that MS@S-NZVI had a significant U(VI) removal rate in simulated wastewater systems. Finally, the removal process of MS@S-NZVI to U(VI) could be divided into three pathways through the XPS technique , adsorption and reduction were the main reaction mechanisms. This study provides a new insight into the utilization of melamine sponge and a prospect for the practical application of S-NZVI in the removal of radionuclide .
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2018
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IF 3.974
Xiaofeng Yi,Fuliang Sun,Zhenhua Han,Fuhao Han,Jiarui He,Minrui Ou,Junjie Gu,Xiaoping Xu
In this work, a novel sodium alginate (SA)/polyvinyl alcohol (PVA)/graphene oxide (GO) hydrogel microspheres were prepared by a simple method. Sodium alginate was physically crosslinked by Ca 2+ ; GO was encapsulated into the composite to strengthen the hydrogels; PVA played a significant role in well dispersing of GO in SA. The SA/PVA/GO (SPG) hydrogels were employed as an efficient adsorbent for removal of Cu (II) and U (VI) from aqueous solution. Batch experiments with the subject of the pH, initial metal ion concentration , competing ions and contact time were investigated. Structure characterization was successfully conducted by FTIR, SEM, EDX, BET and XPS. Furthermore, the sorption kinetics of Cu 2+ and UO 2 2+ followed pseudo-second order model and exhibited 3-stage intraparticle diffusion model. Equilibrium data were best described by Langmuir model and the obtained maximum adsorption capacities of SPG hydrogel microspheres for Cu 2+ and UO 2 2+ were 247.16 and 403.78 mg/g, respectively. The difference in adsorption capacity can be confirmed by the percentage of elements in EDX spectra and the intension of peak of elements in XPS spectra. The SPG sorbent exhibited excellent reusability after 5 adsorption-desorption cycles. All results suggested that the prepared adsorbents could be considered as effective and promising materials for removal of Cu (II) and U (VI) in wastewater.
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SOLID STATE SCIENCES
·
2020
·
IF 2.434
Chao Jiang,Yan Liu,Dingzhong Yuan,Yun Wang,Jinbiao Liu,Jia Wei Chew
In this study, polyphosphazene microspheres (PZS) was prepared by reaction under ultrasonic conditions using hexachlorocyclotriphosphazene (HCCP) and 4,4-dihydroxydiphenyl sulfone (BPS) as raw materials. Phosphoric acid-functionalized microporous carbon materials (denoted as CS-PO 4 ) was further derived from PZS by carbonization and functionalization. The structure of CS-PO 4 was characterized by Fourier Transform Infrared Spectroscopy (FTIR), Scanning Electron Microscopy (SEM) and X-ray photoelectron spectroscopy (XPS). The adsorption properties of CS-PO 4 for uranyl ions in aqueous solution under different conditions (namely pH, contact time, initial concentration and temperature) were investigated. The results indicate that the optimum pH for adsorption was 6 while the equilibrium time was about 40 min. The maximum adsorption capacity was about 1029.8 mg/g, as calculated by the Langmuir model. The comprehensive analysis of the adsorption thermodynamics and kinetics show that the CS-PO 4 can be used to adsorb U(VI) effectively in solution.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Xiaoqin Nie,Yujing Zhang,Yating Jiang,Ning Pan,Chang Liu,Junling Wang,Chunyan Ma,Xue Xia,Mingxue Liu,Hongping Zhang,Xiaoan Li,Faqin Dong
The enrichment and recovery of U(VI) from low-level radioactive wastewater in the process of uranium enrichment is important for the sustainable development of nuclear energy and environmental protection. Herein, a novel amine-aminophosphonate bifunctionalized polyacrylonitrile fiber (AAP-PAN), was prepared for the extraction of U(VI) from simulated and real uranium-containing process wastewater. The AAP-PAN fiber demonstrated a maximum adsorption capacity of 313.6 mg g −1 at pH = 6.0 and 318 K in the batch experiments. During the dynamic column experiment, over 99.99% removal of U(VI) could be achieved by the fiber using multi-ion simulated solution and real wastewater with an excellent saturation adsorption capacity of 132.0 mg g −1 and 72.5 mg g −1 , respectively. It also exhibited an outstanding reusability for at least 5 cycles of adsorption process. The mechanism for U(VI) removal was studied by Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy analysis in the assist of simulation calculation. It suggested that the amine and aminophosphonate groups can easily bind uranyl ions due to U(VI) is more likely to combine with oxygen atoms of C O and P O, respectively.
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PubMed
高影响因子
RADIOCHIMICA ACTA
·
2023
·Vol. 111
·期 12
·895-907
·
IF 1.8
Xiaoyu Yin,Peng Wu,Yufan Zhao,Shilong Shi,Jun Liu,Feize Li,Jiali Liao,Ning Liu,Yuanyou Yang,Tu Lan
The U(VI) sorption behavior on dolomite was systematically investigated in a dilute carbonate solution using batch technique. The distribution coefficients ( K d ) increased with the increasing time and temperature, but decreased with the increase of initial U(VI) concentration and ionic strength. As the initial pH increased from 2.0 to 10.5, the K d values first increased and then decreased, mainly due to the transition from electrostatic attraction to repulsion caused by the changes in U(VI) species. The sorption process was well-described by pseudo-second-order kinetic and Freundlich isotherm models, and was spontaneous, endothermic, heterogeneous, and pH-dependent. In the presence of HA/FA, at low pH, more HAs/FAs were adsorbed on dolomite surface, providing more sorption sites for the positively charged U(VI) species, and promoting the U(VI) sorption. At high pH, more HAs/FAs were dispersed in solution, encapsulating the negatively charged U(VI) species in aggregates, and inhibiting the U(VI) sorption. The promoting and inhibiting effects of HA on the sorption process are obviously stronger than FA. XPS spectra indicated that the surface ‒OH and CO 3 2− on the hydroxylated dolomite and the –OH groups in HA/FA may be involved in U(VI) sorption. The results reported here provide valuable references for further understanding U(VI) migration in geological media.
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Frontiers in Chemistry
·
2019
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IF 3.782
Liu Lijuan,Yang Weiting,Gu Dongxu,Zhao Xiaojun,Pan Qinhe
With the rapid growth of nuclear power generation and fuel processing, the treatment of nuclear industry wastewater has become a major problem, and if not handled properly, it will pose a potential threat to the ecological environment and human health. Herein, a chitosan (CS)/ZIF-8 composite monolithic beads with ZIF-8 loading up to 60 wt% for U(VI) removal was prepared, which can be easily removed after use. It possesses a very high adsorption capacity of 629 mg•g−1 at pH = 3 for U(VI) and a well recyclability is demonstrated for at least four adsorption/desorption cycles. X-ray photoelectron spectroscopy (XPS) was carried out to study the adsorption mechanism between uranium and adsorbent, and the chelation of U(VI) ions with imidazole, hydroxyl, and amino groups was revealed. This work shows that CS/ZIF-8 composite can be used as an effective adsorbent for uranium extraction from aqueous solution, and has a potential application value in wastewater treatment.
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