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RSC Advances · 2021 ·Vol. 11 ·期 38 ·23241-23248 · IF 3.361

Organic acid mediated photoelectrochemical reduction of U(VI) to U(IV) in waste water: electrochemical parameters and spectroscopy

Pingping Wang,Faqin Dong,Dengliang He,Shuxin Liu,Ning Chen,Tingting Huo

The photoelectrochemical reduction of U(VI) is recognized as an economical and effective way to eliminate radioactive pollution. In this study, we construct a α-Fe2O3/TiO2 film electrode-based photoelectrochemical cell to remove U(VI) and recover uranium from aqueous solution. Citric acid and oxalic acid could act as hole scavengers, being favorable for the photocatalytic reduction of U(VI). In the presence of 0.5 mM citric acid and oxalic acid, the uranium removal capacity reached 70% and 58%, respectively, while 24% was achieved for the system in the absence of acid. The XRD, SEM, FT-IR and XPS results revealed that a proportion of U(IV) was also precipitated as surface associated metastudtite. These novel observations have significant implications for the behavior of uranium within engineered and natural environments.

CAS / MDL: 10025-77-1
研究领域: 环境科学 · 材料科学
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WATER RESEARCH · 2025 · IF 12.4

Direct recovery of high-purity uranium from fluoride-containing nuclear wastewater via extraction materials with ensemble Lewis sites and a tandem electrochemical device

Guo Li,Yan Liu,Chi Jiao,Zhengyu Jiang,Juan Zhang,Tao Chen,Tao Lin,Rong He,Wenkun Zhu,Xiangke Wang

Electrochemical uranium extraction from real nuclear wastewater with a high concentration of fluoride ions (F-) represents a promising strategy for the efficient treatment of radioactive wastewater and the recovery of the valuable uranium resource. However, the current progress suffers from the interference of extremely high concentration of F- and undesired purity of the final uranium product. Herein, we constructed the neighboring ensemble Lewis acid-base pair sites (ensemble Lewis sites) in bismuth oxides as the extraction material, which was integrated into a designed tandem electrochemical device for efficient recovery of high-purity uranium from real nuclear wastewater. The mechanistic study revealed that the ensemble Lewis sites dramatically enhance the binding of all dominant uranyl fluoride (UO2Fx) species through the simultaneous strengthened chemical bonds with U, O, and F atoms. Besides, the tandem electrochemical device rationally controlled the reaction period to U3O8, avoiding the undesired crystalline transformation to K2U2O7. Through 3 h electrolysis in 1 L of real nuclear wastewater, the extraction efficiency of uranium reached 99.9 % with only 2.2 % impurities of alkali metals in extracted uranium product, outperforming the previous work. This study offers an effective method for the recovery of uranium resources in real nuclear wastewater.

CAS / MDL: 7697-37-2 7664-93-9
研究领域: 材料科学 · 环境科学 · 核能工程
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2022 · IF 5.518

An efficient and high-capacity porous functionalized-membranes for uranium recovery from wastewater

Yun Xue,Jiaqi Chen,Peng Liu,Jianzhang Gao,Yunyang Gui,Wanting Cheng,Fuqiu Ma,Yongde Yan

In order to satisfy the increasing needs for sustainable development of the nuclear energy industry, it is critical to vigorously develop efficient materials for uranium separation and recovery from wastewater. In this work, novel amidoxime-functionalized membranes (PAO membranes) were successfully synthesized via a facile one-step non-solvent induce phase separation rather than as-reported synthesized approaches that needed complicated additives or harsh reaction conditions. The pore channels provided large specific surface areas and massive binding sites, and the bulk-shape membrane was convenient for collection. Removal of uranium as a function of initial pH, reaction time, initial concentrations of U(VI), and temperature was studied. The maximum adsorption capacity of the PAO membranes toward U(VI) calculated from the Langmuir model was up to 641.72 mg·g −1 at pH 5 and 298 K. Thermodynamic studies indicated that the enrichment of U(VI) was a spontaneous and endothermic process. The removal percentage of uranium reached 86.50% in simulated wastewater in the case of multiple coexisting metal ions . In addition, the scanning electron microscope (SEM), Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS) results confirmed that the abundant adsorption sites of the PAO membranes were responsible for the efficient immobilization of uranium by forming chelating species, especially amidoxime groups and carboxyl groups. This work presents a novel strategy for mass production of a new generation of high-efficiency adsorbents for uranium-containing wastewater treatment in the future.

研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Alkaline ion exchange fibers constructed by UV-induced radical polymerization for efficient uranium recovery from wastewater and seawater

Bingying Li,Jingyuan Liu,Qi Liu,Jiahui Zhu,Jing Yu,Shusen Chen,Yan Song,Rumin Li,Jun Wang

Extracting uranium from natural seawater and wastewater is an effective approach to alleviating the current energy crisis and promoting green development in the nuclear industry. Herein, novel collagen fibers (CFs)-based strong alkaline ion-exchange fibers (CFs-SAA-IEF) were prepared through free radical polymerization initiated by ultraviolet light irradiation and an amination reaction. The CFs-SAA-IEF fibers exhibited an impressive adsorption capacity of 675.68 mg g −1 at pH = 8, along with exceptional selectivity, achieving a K d value of 1.24 × 10 4 mL g −1 . Notably, due to the ion-exchange effect, CFs-SAA-IEF showed rapid adsorption kinetics, achieving a uranium removal rate of 85.9 % within 120 min. Meanwhile, the incorporation of quaternary ammonium groups imparted the adsorbents with excellent antibacterial properties even in complex aqueous environments. In addition, CFs-SAA-IEF demonstrated an exceptional adsorption performance and a high removal rate of uranium in wastewater and seawater by fixed-bed column adsorption system. Based on the XPS spectra and DFT calculation, uranyl ions are captured by the adsorbents through chemisorption, involving the ion exchange of chloride ions with uranyl ion complexes. In summary, the CFs-SAA-IEF fibers are promising candidates for the efficient recovery of uranium from seawater and wastewater.

CAS / MDL: 109-99-9
研究领域: 环境科学 · 材料科学
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GREEN CHEMISTRY · 2019 ·Vol. 21 ·期 3 ·649-657 · IF 9.405

Solvent- and catalyst-free synthesis of an azine-linked covalent organic framework and the induced tautomerization in the adsorption of U(VI) and Hg(II)

Xing Li,Yue Qi,Guozong Yue,Qianxun Wu,Yang Li,Meicheng Zhang,Xinghua Guo,Xiaofeng Li,Lijian Ma,Shoujian Li

A green and facile solvent- and catalyst-free method, without inert gas protection and/or mechanical grinding to synthesize an azine-linked covalent organic framework (ACOF) with high efficiency, was proposed for the first time. Characterization techniques and experimentations show that the as-synthesized ACOF has high crystallinity and superior physical and chemical stability and exhibits good adsorption performance for both radioactive heavy metal U(VI) and ordinary heavy metal Hg(II), with adsorption capacities of 169 mg g−1 for U(VI) and 175 mg g−1 for Hg(II), which makes the ACOF a potential adsorbent material for heavy metal removal and uranium recycling. Tautomerization between the enol-form and keto-form was verified in the structure of the ACOF which can be induced by the adsorption of metal ions and also affect the adsorption properties simultaneously. It was found that tautomerization from the enol-form to keto-form was promoted in the adsorption, which can be ascribed to the better coordination ability of CO in the keto-form towards the target metal ion, while the selectivity of the ACOF towards U(VI) increases with the decreasing solution pH and reaches 96.2% when the pH is 1.5, which is due to the tautomerization from the keto-form to enol-form under acidic conditions and the consequent size-matching effect. The study on tautomerization in solid materials is rarely reported and is of great importance for deep understanding of the relationship between material structures and properties. The synthesis strategy proposed in this paper provides references for the convenient, efficient and green synthesis of COFs.

研究领域: 材料科学 · 环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Self-locomotive composites based on asymmetric micromotors and covalently attached nanosorbents for selective uranium recovery

Kaiwen Yang,Fan Wu,Xincheng Yan,Jianming Pan

Nanosized sorbents are widely used for uranium (VI) recovery due to their high specific surface area, but the research on the integration of micromotors with nanosorbents to establish self-locomotive composites is still worth exploring. Thus, self-locomotive composites PS@PDA@Ag/SiO 2 -AO (PPA/SA) based on asymmetric micromotors and covalently attached nanosorbents were designed for selective uranium recovery. Pickering emulsion, as an important micro-reactor, was firstly adopted to prepare Janus microspheres with chemically distinct structure (PS@PDA@Ag), on which one hemisphere was loaded with catalytic silver (Ag) nanoparticles. Then, amidoxime (AO) decorated SiO 2 nanospheres were covalently attached onto another hemisphere of PS@PDA@Ag, anisotropic configuration of as-prepared PPA/SA avoided the overlap of catalytic and binding sites. The self-propelled motion of PPA/SA induced by asymmetrical bubble evolution by H 2 O 2 was observed, and the maximum speed was about 25 μm s −1 in case of 5 % H 2 O 2 . The uranium adsorption onto PPA/SA achieved 92 % of the equilibrium amount (29.31 mg g −1 ) in the first 20 min, and this value increased to 38.71 mg g −1 under the condition of H 2 O 2 , suggesting that autonomous movement achieves rapid mixing and mass transportation. The maximum adsorption amount ( Q m ) is 114.0 mg g −1 at 298 K according to the Langmuir model. In addition, PPA/SA exhibited remarkable selectivity for uranium even in the presence of large amounts of Na + , Mg 2+ , K 2+ , Ca 2+ and other ions in the simulated seawater solution.

研究领域: 材料科学 · 环境科学
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NEW JOURNAL OF CHEMISTRY · 2024 ·Vol. 48 ·期 43 ·18546-18557 · IF 2.7

Short-range conjugated nitrogen-rich porous polymers for uranium(VI) photocatalysis

Jiaxin Hu,Qihang Sun,Baoyu Li,Yunwen Liao,Juan Zhang,Jinming Chang,Hejun Gao,Hongquan Fu

The recovery of uranium from uranium-containing wastewater is crucial for the nuclear energy industry. Despite the effectiveness of photocatalytic reduction of uranium from U(VI) to U(IV) in treating uranium-containing wastewater, conventional organic conjugated semiconductors face challenges due to their high cost and reliance on inert gases. This study introduces an economical and eco-friendly approach using trimeric cyanuric chloride to construct a nitrogen-rich porous polymer (Py-NPP) with a short-range conjugated π unit and a pyrrole end-cap. Py-NPP demonstrated a remarkable removal efficiency of 93% in a 100 mg L−1 U(VI) solution, even reaching 89% under ambient air. Py-NPP demonstrated good stability, with a uranium removal rate still over 80% after being cycled four times. Moreover, it still exhibited a good removal rate under 500-fold salt concentration. The nitrogen-containing functional groups enhanced chelation with U(VI), while the triazine structure and short-range conjugation of the π unit boosted photocatalytic activity, facilitating charge separation and transfer. This study offers a promising strategy for efficient U(VI) reduction using short-range conjugated catalysts under ambient conditions.

研究领域: 材料科学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Ferrocene-based 2D metal–organic framework nanosheet for highly efficient photocatalytic seawater uranium recovery

Shilei Zhao,Tiantian Feng,Meng Cao,Tao Liu,Yihui Yuan,Ning Wang

Sustainable uranium supply is critical for the long-term development of nuclear energy. The photocatalytic reduction of soluble hexavalent uranium to insoluble tetravalent uranium using photocatalysts has been recognized as a highly promising method for uranium recovery. However, existing photocatalysts face limitations such as restricted visible-light absorption and poor charge transfer capability, which hinder their photocatalytic uranium recovery performance. In this work, 1,1′-ferrocene dicarboxylic acid (FcDA) was introduced to synthesize the photocatalyst Zr-Fc-MOF 3 . The incorporation of FcDA broadened the visible light absorption range and reduced the band gap of Zr-Fc-MOF 3 , thereby enhancing electron-hole pair separation and carrier transport efficiencies. Moreover, the two-dimensional (2D) nanosheet structure of Zr-Fc-MOF 3 provided a large surface area, allowing full exposure of active sites. Additionally, Fe(II) in FcDA generated photoelectrons upon light excitation to facilitate uranium reduction, and the recyclable redox behavior of Fe(II) conferred high reusability of the photocatalyst. Consequently, Zr-Fc-MOF 3 demonstrated a high photocatalytic uranium recovery capacity of 8.29 mg g −1 over 10 days in natural seawater (NSW), with a uranium recovery rate of 0.829 mg g −1 d −1 , surpassing most other photocatalysts applied in NSW. These findings suggest that designing 2D nanosheet materials with ligands capable of efficient photoelectron generation is a promising approach for developing high-performance uranium recovery photocatalysts.

CAS / MDL: 68-12-2 10026-11-6
研究领域: 材料科学 · 环境科学 · 核能技术
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ACS Omega · 2022 · IF 4.132

Enhancement of Uranium Recycling from Tailings Caused by the Microwave Irradiation-Induced Composite Oxidation of the Fe–Mn Binary System

Qingxiang Wang,Tao Huang,Jing Du,Lulu Zhou

The extraction of uranium (U)-related minerals from raw ore sands via a leaching procedure would produce enormous amounts of tailings, not only causing radioactivity contamination to surroundings but also wasting the potential U utilization. Effective recycling of U from U tailings is propitious to the current issues in U mining industries. In this study, the influence of the composite oxidation of Fe(III) and Mn(VII) intensified by microwave (MW) irradiation on the acid leaching of U from tailings was comprehensively explored in sequential and coupling systems. The U leaching activities from the tailing specimens were explicitly enhanced by MW irradiation. The composite oxidation caused by Fe(III) and Mn(VII) further facilitated the leaching of U ions from the tailing under MW irradiation in two systems. Maximum leaching efficiencies of 84.61, 80.56, and 92.95% for U ions were achieved in the Fe(III)-, Mn(VII)-, and Fe(III)–Mn(VII)-participated coupling systems, respectively. The inappropriateness of the shrinking core model (SCM) demonstrated by the linear fittings and analysis of variance (ANOVA) for the two systems explained a reverse increase of solid cores in the later stage of leaching experiments. The internal migration of oxidant ions into the particle cores enhanced by MW accelerated the dissolution of Al, Fe, and Mn constituents under acidic conditions, which further strengthened U extraction from tailing specimens.

研究领域: 环境科学 · 核工程 · 化学工程 · 材料科学
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JOURNAL OF MEMBRANE SCIENCE · 2025 · IF 9

Biofouling-resistant amidoxime-functionalized chitosan membranes enable efficient uranium recovery from salt-lake water

Wei Luo,Sifan Gao,Linping Yan,Xuepin Liao,Bi Shi

The limited availability of terrestrial uranium resources poses significant challenges to the development of nuclear energy. Extracting uranium from Salt Lake water offers a new solution to address the shortage of uranium resources. This study used chitosan, a naturally adsorptive material, to create chitosan microporous membranes (CS) with polyethylene glycol as a porogen. Subsequently, a novel amidoxime-based chitosan microporous membrane adsorbent (CS-AO) was developed based on CS for uranium extraction from Salt Lake water. The CS-AO membrane's hydroxyl, amino, and amidoxime groups work synergistically to provide multiple binding sites, significantly enhancing its binding capacity for UO 2 2+ . Under optimal conditions (initial concentration 3.0 mmol L −1 , temperature 323 K, pH 6), the adsorption capacity reached 2.84 mmol g −1 , with rapid adsorption/desorption rates and good selectivity. At a uranium feed concentration of 0.05 mmol L −1 and flow rate of 1.0 mL min −1 , the treatment capacity was 1046.93 L m −2 . Moreover, when applied to actual brine collected from the Chaerhan Salt Lake in Golmud, Qinghai, China for uranium extraction, CS-AO achieves an extraction rate of 79.6 %. Additionally, CS-AO showed over 90 % antibacterial effects against E. coli and S. aureus , with excellent stability, making it suitable for long-term Salt Lake uranium extraction.

CAS / MDL: 9012-76-4
研究领域: 核能 · 环境科学 · 材料科学 · 化学工程 · 吸附技术
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Bifunctional Phosphorylcholine-Modified Adsorbent with Enhanced Selectivity and Antibacterial Property for Recovering Uranium from Seawater

Zeng Huang,Hao Dong,Na Yang,Hao Li,Ningning He,Xirui Lu,Jun Wen,Xiaolin Wang

The recovery of uranium from seawater is of great concern because of the growing demand for nuclear energy. Though amidoxime-functionalized adsorbents as the most promising adsorbents have been widely used for this purpose, their low selectivity and vulnerability to biofouling have limited their application in real marine environments. Herein, a new bifunctional phosphorylcholine-modified adsorbent (PVC–PC) is disclosed. The PVC–PC fiber is found to be suitable for use in the pH range of seawater and metals that commonly coexist with uranium, such as alkali and alkaline earth metals, transition metals, and lanthanide metals, have no obvious effect on its uranium adsorption capacity. PVC–PC shows better selectivity and adsorption capacity than the commonly used amidoxime-functionalized adsorbent. Furthermore, PVC–PC fiber exhibits excellent antibacterial properties which could reduce the effects of biofouling caused by marine microorganisms. Because of its good selectivity and antibacterial property, phosphorylcholine-based material shows great potential as a new generation adsorbent for uranium recovery from seawater.

研究领域: 材料科学 · 环境工程 · 核能
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Journal of Water Process Engineering · 2022 · IF 7.34

Bioinspired grafting of peptide and NH2-AO to construct antifouling fiber membranes for fast uranium recovery from wastewater and seawater

Bochen Li,Yuefei Wang,Guoping Xiao,Se Shi,Peiqi Zhao,Ruxi Feng,Haiquan Zhang,Yihui Yuan,Hui Wang,Tao Liu,Ruizhi Zhang,Ning Wang

Uranium is an important nuclear element, and its efficient recovery is of great significance to nuclear industry and to nuclear safety. Herein, we rationally design robust antifouling fiber membranes (Anti-NH 2 -AO FMs) by facilely grafting two novel ligands on porous surfaces. The efficient ligands, i.e., NH 2 -AO and GSH, endow the membranes with rapid U-capture rate, good hydrophilicity and antifouling ability. Anti-NH 2 -AO FMs display porous fiber network structure, good flexibility, and high mechanical strength (9.0 MPa). The uranium capture rate reaches up to 167 mg g −1  h −1 in the first two hours, and they can reduce uranium to 11 ppb in 2 ppm uranium-contaminated water, which is below the drinking water limit. Furthermore, Anti-NH 2 -AO FMs still exhibit very high seawater permeability (6186 L m −2  h −1  bar −1 ) and flux recovery ratio (95.12 %) after three seawater fouling cycles. The imaging tests visually demonstrate their antiadhesion to the bacteria. In addition, they have good selectivity and long service life (10 cycles of adsorption-desorption). Kinetics models and XPS analyses illustrate the uranium adsorption mechanisms. Compared with the current membranes and fibers, the Anti-NH 2 -AO displays the advantages of exceptional properties and easy preparation, and we believe that it possesses great potential in the practical uranium recovery.

CAS / MDL: 1668-00-4 77-86-1
研究领域: 材料科学 · 环境工程 · 核能技术
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