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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

A reductive strategy with ultrahigh selectivity for sequential recovery of uranium from radioactive wastewater

Jianzhang Gao,Jiaqi Chen,Huitao Lv,Xingan Feng,Shitao Liao,Zhidong Wen,Yongde Yan,Yun Xue,Fuqiu Ma

Uranium is valuable metal, and it is of great significance to develop a simultaneous separation process of uranium and cesium from radioactive wastewater. Herein, a process was designed to separate sequentially uranium and cesium from wastewater. By comparing the limiting ability of OH − and CO 3 2− to Co 2+ , Cd 2+ , and Sr 2+ ions, it was found that CO 3 2− could effectively limit the above ions to the solid phase. The result of X-ray photoelectron spectroscopy (XPS) and species analysis revealed that the restriction was achieved through complexation. Through this property, more than 99.9 % of cobalt and cadmium were limited in the solid phase, and U-Cs co-separation was realized. Furthermore, the results of cyclic voltammetry and XPS indicated that U(VI) could be reduced in the liquid phase, but Cs(I) could not, which was the basis for uranium and cesium separation. And more than 99.5 % of uranium was separated from cesium by the electrochemical separation process. Simultaneously, effective separation of uranium and cesium under different pHs has been achieved via selective uranium leaching using carbonate. The co-separation combined with electrochemical separation realized the recovery of pure uranium products, indicating a large potential for realizing uranium resources in wastewater.

CAS / MDL: 7646-79-9
研究领域: 环境科学 · 核化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Ammonium phosphomolybdate-modified UiO-66 as an efficient adsorbent for the selective removal of 137Cs from radioactive wastewater

Siyu Liu,Jianhua Zu,Gang Han,Xiaohan Pan,Yi Xue,Jingjie Diao,Qing Tang,Mingjie Jin

137 Cs is a radioactive pollutant in the production of wastewater from nuclear power plants. In this study, a rapid and simple in-situ synthesis new method was employed to prepare a novel AMP-functionalized UiO-66 composite material for the selective capture of 137 Cs from low-level radioactive wastewater. Characterization techniques such as SEM-EDS, FTIR, XRD, TG, and BET were used to confirm the successful loading of AMP on the surface of UiO-66. UiO-66/AMP showed a good removal effect in pH4-11. At pH7, the effects of different parameters, such as the initial Cs concentration, the ratio of the amount of adsorbent to the volume of solution, and the adsorption time were investigated. The adsorption efficiency is 96.7%, the maximum adsorption capacity is 94.9 mg/g and has fast adsorption kinetics (90% Cs + removal within 5 min). The adsorption data conformed to the pseudo-second-order kinetic model and Langmuir isotherm model, suggesting a monolayer homogeneous adsorption process. XPS helps confirm that the adsorption mechanism is the ion exchange between Cs + and NH 4+ ions. Particularly, in the adsorption experiments of 137 Cs, UiO-66/AMP demonstrated good selectivity (K d Cs : 5.8 × 10 3  ∼ 1.26 × 10 4 mL/g) towards trace Cs + in a mixed ion solution with a molar ratio of 1 (Cs): 2.18 × 10 15 (Na): 4.6 × 10 14 (K): 2 × 10 14 (Mg): 2 × 10 14 (Ca), indicating its potential for selective capture of 137 Cs from low-level liquid waste (LLLW).

CAS / MDL: 10026-11-6
研究领域: 环境科学 · 核化学与放射化学
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION · 2020 · IF 4.966

The separation of radionuclides and silicon from boron-containing radioactive wastewater with modified reverse osmosis membranes

Boxian Chen,Suping Yu,Xuan Zhao

The ability to reuse boron and minimize the volume of radioactive waste could be accomplished with modified reverse osmosis (RO) membranes. RO membranes were fabricated via polyethylenimine (PEI) grafting to separate silicon and radionuclides from boron-containing radioactive wastewater . The positively charged RO membrane promoted more efficient removal of nuclides and silicon while the rejection of boron declined from 55.88 % to 41.71 % after modification. Compared with virgin RO membrane, the SF B-Si , SF B-Cs , and SF B-Co of the modified RO membranes increased from 6.02, 5.16, and 12.62–29.52, 61.91, and 547.15, respectively. SF B-Si , SF B-Cs , and SF B-Co of the simulated RO system with modified RO membranes further increased to 156.96, 1068.12, and 83617.88, respectively. As a result, permeate water with 433.92   mg   L −1 boron, 0.04   mg   L −1 silicon, 1.62   μg · L −1 Cs(I), and 0.02   μg · L −1 Co(II) was obtained, which could satisfy radionuclide treatment requirements and allow for the reuse of boron. Overall, modified RO membranes would be able to reuse boron and minimize the volume of discharge of radioactive wastewater.

研究领域: 环境科学 · 材料科学 · 核能工程
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JOURNAL OF SOLID STATE CHEMISTRY · 2021 · IF 3.498

Preparation of phosphorylated iron-doped ZIF-8 and their adsorption application for U(VI)

Jiaying Pei,Zhongsheng Chen,Youqun Wang,Bo Xiao,Zhibin Zhang,Xiaohong Cao,Yunhai Liu

In this study, a 10%Fe-ZIF-8-300-PO 4 adsorbent was synthesized and its adsorption performance for U(VI) was investigated comprehensively. It was found that after a series of operations such as Fe doping, thermal activation and phosphorylation, the adsorption performance for U(VI) can be significantly improved on the basis of maintaining the skeleton characteristics of ZIF-8. The results showed that the optimal Fe-doping amount and thermal activation temperature was 10% and 300°C, respectively. The adsorption of U(VI) on 10%Fe-ZIF-8-300-PO 4 reached equilibrium within 60 ​min, and conformed to pseudo-second-order kinetic equation. Furthermore, a maximum saturated adsorption capacity of 691.83 ​mg/g was achieved. The above results demonstrated that 10%Fe-ZIF-8-300-PO 4 may be used to efficiently remove U(VI) from uranium-containing radioactive waste water.

研究领域: 环境科学 · 材料科学
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Surfaces and Interfaces · 2024 · IF 5.7

Reverse osmosis membrane with crown ethers decoration for enhanced radionuclides sieving

Yi Wang,Jianlong Wang,Li'an Hou

Reverse osmosis (RO) membranes have been widely applied in the increasingly discharged radioactive wastewater treatment . However, conventional RO membranes suffer from the issues of the limited nuclides rejections and the relatively low water permeance. In this work, a new type of RO membrane with decoration of crown ethers (15C5 and 18C6) was prepared via an interfacial polymerization process to remove the radionuclide-contaminated components. Due to the special hollow structure of crown ethers (CEs) and the hydrogen bonding within the amidogen, the obtained MPD@15C5-TMC and MPD@18C6-TMC membranes exhibited smoother surfaces and thinner polyamide active layers than the pristine MPD-TMC membrane. The optimized MPD@15C5-TMC and MPD@18C6-TMC RO membranes presented excellent pure water permeances up to 2.16 and 2.91 L m −2 h −1 bar −1 , and maintained high rejections towards Cs + , Sr 2+ and Co 2+ , respectively. Furthermore, the membrane possessed a remarkable operational stability and an excellent anti-fouling property. These results confirmed the possibility of adopting crown ethers for RO membrane fabrication and verified their great potential for the practical application in removing radioactive elements from wastewater.

CAS / MDL: 68131-04-4
研究领域: 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

Highly efficient capture of TcO4-/ReO4- by imidazolium ionic liquid supported silica materials prepared by radiation induced RAFT-mediated graft polymerization technology

Xiaoyang Liu,Na Zhang,Zhen Dong,Jifu Du,Lifang Peng,Long Zhao,Miao Yang

Technetium ( 99 Tc) is a main long-lived radionuclide of nuclear waste, which poses a great threat to the environment and human health. The reasonable disposal of 99 Tc is vital important. In this paper, a series of novel materials (SMILR m , m = 0, 1/500, 1/200, m is the molar ratio of IL to RAFT reagent) was synthesized by radiation-induced grafting combined with reversible addition-fragmentation chain transfer (RAFT) polymerization. The adsorption performance of SMILR m to 99 Tc were investigated. The graft polymerization process is controlled by the RAFT reagent, resulting in a restricted dispersion of SMILR m molecular weight. With the increase of RAFT reagent content, the grafting yield (GY) decreased. The addition of RAFT reagent increases the specific surface area of the adsorbent, accelerates the adsorption rate, increases the adsorption capacity, but reduces the adsorption selectivity. Especially, the adsorption of SMILR 0 was a single step adsorption and obeyed Langmuir adsorption model, while SMILR m (1/500, 1/200) showed a stepwise adsorption isotherm model. SMILR m exhibited excellent recyclability and could efficiently capture Re O 4 - from a simulated Beishan groundwater in dynamic experiments. Finally, XPS and FT-IR analysis confirmed that the adsorption was an ion exchange mechanism. The results showed that SMILR m are suitable for the effective removal of Re O 4 - / T c O 4 - from radioactive wastewater with complex composition.

CAS / MDL: 112926-00-8 2530-85-0
研究领域: 环境科学 · 核化学与放射化学
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY · 2019 ·Vol. 95 ·期 4 ·1085-1092 · IF 2.659

The application of polyethylenimine grafting reverse osmosis membrane in treating boron-containing low-level radioactive wastewaters

Boxian Chen,Ding Chen,Xuan Zhao

BACKGROUND Reverse osmosis (RO), which is widely utilized in wastewater treatment, has been proven to be an effective tool for ion separation with high salts rejection. However, owing to the extremely low concentration of nuclides in boron-containing low-level radioactive wastewaters (LRWs), there is a significant reduction in rejection of nuclides by using commercial RO membranes. In this study, in order to obtain higher nuclides rejection under trace-level condition, novel polyamide RO membranes were fabricated by grafting polyethylenimine (PEI) with different molecular weights on commercial RO membrane surfaces. RESULTS The properties of PEI-modified membranes were analyzed, such as surface charge, morphology and hydrophilicity. The results showed that zeta potential at pH 7 increased from −22.89 mV to 20.19 mV, which indicated that surface charge altered from negative to positive. Meanwhile, hydrophilicity of membranes was improved since the contact angle decreased from 65° to 36°. The decontamination factor (DF) of cesium(I) increased from 11.69 to 114.23 and the DF of cobalt(II) increased from 28.62 to 3306.88. CONCLUSION The laboratory-scale experiments with cross-flow demonstrated the effective rejection of nuclides without obvious membrane flux loss of PEI-modified membranes. In addition, PEI-modified membranes offered a stable nuclides removal under high-level background boron and various pH conditions, which demonstrated a possible application in boron-containing LRW treatment. © 2019 Society of Chemical Industry

研究领域: 环境科学 · 材料科学
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Journal of Cleaner Production · 2019 · IF 6.395

Optimization analysis and mechanism exploration on the removal of cesium and the solidification of secondary residue wastes in electrokinetics

Fangzhu Xiao,Tao Huang,Shuwen Zhang,Longfei Liu,Cheng Wang,Guowen Peng,Shuya He

The fallout of the radioactive nuclide cesium (Cs) has posed its potential environmental threat to human health and ecosystem during the Fukushima accident. Thus, Cs decontamination from radioactive wastewater is strongly required for treating similar occurrences. In this work, a coupling method was applied to achieve Cs + removal and solidification in one conducting system. Ammonium molybdophosphate (AMP) was loaded to blast furnace slag (BFS) particles for the preparation of adsorbent (BFS-AMP) and binder. The maximum adsorption capacity of BFS-AMP for Cs + was 23.36 mg/g obtaining at the pH of 8 and the initial concentration of 500 mg/L in the equilibrium adsorption experiments. Cs + uptake confirmed to the pseudo-first-order kinetic model . Electrokinetics (EK) not only increased the adsorption capacity of BFS-AMP also enhanced the migration of Cs + ions from the anode to cathode in the electrolyzer . The transfer of Cs + ions from liquid to solid in the electrolyzer was controlled by both voltage gradients and flow rates. The solidification of EK-treated BFS-AMP mortar was mainly dominated by the mass ratios (wt.%) of alkali activator to adsorbent and the initial pH values. Cs + leaching from the solidified products of EK-treated BFS-AMP mortars ranged from approximately 1.18 × 10 −7 to 9.54 × 10 −6  g cm −2 ∙d −1 . The electromigration , geopolymer stabilization, and hydration encapsulation were concluded as the main incorporation mechanisms for Cs + ions transferring from the stock solution into the BFS-AMP-based solidification in the electrolyzer.

CAS / MDL: 7722-76-1 12054-85-2
研究领域: 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

In situ chemical oxidation-grafted amidoxime-based collagen fibers for rapid uranium extraction from radioactive wastewater

Yi Tang,Jibo Zhou,Wei Luo,Xuepin Liao,Bi Shi

The development of an amidoxime (AO)-based biomass adsorbent offers a solution for uranium extraction from radioactive wastewater and seawater. It also provides a strategy for realizing environmental safety and resource sustainability. Here, an AO-based collagen fiber (CF) adsorbent (AO-CF) was fabricated via in situ oxidative grafting. The fibrous morphology enables AO-CF to realize faster adsorption rate and higher adsorption capacity. During batch adsorption, the adsorption capacity of AO-CF was 0.877 mmol g −1 (234.16 mg g −1 ) at 318 K and pH 5.0 when the initial concentration of UO 2 2+ was 2.5 mmol/L, while the adsorption capacity of AO-CF at pH 8.2 was 1.128 mmol g −1 (301.18 mg g −1 ). Moreover, AO-CF exhibited high selectivity for UO 2 2+ in bilateral mixed solutions, including NH 4 + , Zn 2+ , Cr 3+ , Mg 2+ , Al 3+ , Ca 2+ , Ni 2+ , Ba 2+ , and Sr 2+ . Furthermore, AO-CF demonstrated higher adsorption capacity of UO 2 2+ than its major competing element, namely, VO 2+ , in seawater. The adsorption behavior of UO 2 2+ in the nuclear fuel preparation wastewater on the AO-CF column showed that the breakthrough point was approximately 175.0 bed volume (BV), and the AO-CF column could be rapidly regenerated by using only 3.0 BV of 0.1 mol/L HCl solution, indicating excellent reapplication ability. This work presents a new technology for the synthesis of highly efficient adsorbents for the recovery of UO 2 2+ from radioactive wastewater.

CAS / MDL: 107-13-1 97-65-4
研究领域: 环境科学 · 材料科学
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SCIENCE OF THE TOTAL ENVIRONMENT · 2024 · IF 8.2

Construction of MIL-100(Fe)-DMA material for efficient adsorption of Sr and Cs ions from radioactive wastewater

Guohui Wang,Qixin Zhang,Lailai Qin,Kaixuan Tan,Chunguang Li,Lianshun Li,Tinggui Yang,Xiaojuan Liu

A novel metal-organic framework (MOF) material, MIL-100(Fe)-DMA, was synthesized using the solvothermal method. The structure of the MOF was characterized using scanning electron microscopy-energy dispersive X-ray spectroscopy, N 2 adsorption–desorption isotherms, X-ray diffraction analysis, Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy, and Mössbauer spectroscopy. Batch adsorption experiments were performed to investigate the effects of initial Sr 2+ and Cs + concentrations, adsorption time, pH, and coexisting cations on the adsorption performance of the material. The adsorption mechanism was further elucidated using adsorption kinetics and isotherm models. The results indicated that the adsorption of Sr 2+ and Cs + does not significantly affect the MOF material structure. As reaction time and initial ion concentration increased, the adsorption capacity of MIL-100(Fe)-DMA for Sr 2+ and Cs + increased rapidly and then gradually reached equilibrium. Optimal adsorption occurred under alkaline conditions, with maximum adsorption capacity observed at pH = 8. The adsorption process for Sr 2+ and Cs + was well described by the pseudo-second-order kinetic model, the Weber–Morris model, and the Langmuir adsorption isothermal model. The adsorption process was mainly identified as monolayer chemical adsorption, influenced by multiple factors. Characterization combined with density functional theory calculations revealed that the unsaturated carboxylic acid groups on the surface of the MOFs play a crucial role in the interaction with Sr 2+ and Cs + .

研究领域: 材料科学 · 环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2020 · IF 5.774

Radioactive wastewater treatment with modified aromatic polyamide reverse osmosis membranes via quaternary ammonium cation grafting

Boxian Chen,Ding Chen,Xuan Zhao

With the growing application of nuclear power, development of methods for the treatment of radioactive wastewater has become increasingly important. In this study, a positively charged aromatic polyamide reverse osmosis (RO) membrane was prepared using a quaternary ammonium salt (2, 3-epoxypropyltrimethylammonium chloride, EPTAC) grafting to improve nuclide removal efficiency. After modification, the zeta potential of the RO membrane surface increased from −22.89 mV to 21.20 mV in neutral conditions. The positively charged RO membrane promoted more efficient removal of nuclides when compared with the original RO membrane. The decontamination factor (DF) of cesium (I) increased from 11.69 to 151.12 and the DF of cobalt (II) increased from 28.62 to 1670.84. In addition, the surface properties of the modified RO membrane were measured, including hydrophilicity, chemical elements, and morphology. The results of these analyses demonstrated that the hydrophilicity of the membrane was significantly improved as the water contact angle decreased from 65° to 10°. The analysis also demonstrated that the EPTAC-modified RO membrane had a stable nuclide DF under different pH conditions. A brief comparison of the DF of nuclides between commercial RO membranes and modified membranes demonstrated a potential application of EPTAC-modified RO membranes for the treatment of radioactive wastewater from nuclear power plants.

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

Anti-biofouling multi-modified chitosan/polyvinylalcohol air-blown nanofibers for selective radionuclide capture in wastewater

Hongli Lyu,Yao Han,Rui Zhang,Yundi Wu,Xilong Wu

Significant amounts of radioactive wastewater including uranium are discharged into the environment as a result of the expansion of large-scale nuclear power. Due to uranium's toxicity and bioaccumulation, it is crucial to develop efficient and long-lasting adsorbents with functional groups for improving the selective removal of U(VI). By successfully introducing amidoxime and phosphate groups into quaternary ammonium chitosan (QCS-AO/P, i.e., QAP), an antimicrobial composite nanofiber adsorbent (PQAP) composed of polyvinyl alcohol (PVA) and the as-prepared QAP was synthesized via the solution blow spinning technology (SBS) technique for the highly efficient recovery of uranium from wastewater. The influence of initial pH, contact time, and sorbent composition on the uranyl ion absorption and the antibacterial assay was studied. The PQAP composite fiber mat had the highest adsorption capacity of uranyl ions at pH 8 (559.26 mg/g), and showed excellent antibacterial activities. After six adsorption–desorption cycles, PQAP still retained a high uranium adsorption capacity of 420 mg/g and elimination efficiency (84%). The novel integrated sorption and antibacterial strategy provides new insights for highly efficient treatment of radioactive wastewater.

研究领域: 环境科学 · 材料科学 · 核工程
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