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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Effective adsorption and immobilization of Cr(VI) and U(VI) from aqueous solution by magnetic amine-functionalized SBA-15

Fenglei Liu,Anjie Wang,Miao Xiang,Qingyuan Hu,Baowei Hu

Herein, a magnetic amine-functionalized mesoporous silica SBA-15 (Fe 3 O 4 @SBA-15-PDA/HBP-NH 2 ) adsorbent was fabricated by loading Fe 3 O 4 nano-particles on amino-terminated hyperbranched polymers (HBP-NH 2 ) functionalized SBA-15 and exploited for chromium (VI) and uranium (VI) elimination. The morphologies and microstructures of as-obtained materials were observed using different physicochemical and spectroscopic techniques. Meanwhile, batch experiments were performed to investigate the impacts of various water environment conditions on removal process including solution pH, equilibrium time and temperatures. The maximum adsorption capacities of U(VI) and Cr(VI) on Fe 3 O 4 @SBA-15-PDA/HBP-NH 2 reached up to 77.4 mg/g and 66.5 mg/g under optimal water environment conditions. Moreover, the characterization analysis manifested that removal of U(VI) was fulfilled through the surface complexation with amino and phenolic hydroxyl groups, while Cr(VI) were firstly electrostatically adsorbed, and subsequently reduced to less toxic Cr(III) by phenolic hydroxyl groups. These findings demonstrated that this new magnetic amine-functionalized SBA-15 could be considered as valuable materials in environmental cleanup.

研究领域: 环境科学 · 材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Ti3C2Tx/Cd0.8Zn0.2S composites constructed of Schottky heterojunction for efficient photocatalytic reduction of U(VI)

Yun Tian,Luowen Xu,Shuo Ning,Changfu Wang,Yun Wang,Hao Jiang,Dingzhong Yuan,Fengtao Yu,Yan Liu

Photocatalysis has emerged as a extremely promising green technology for the treatment of uranium-containing wastewater. This study focuses on the fabrication of Ti 3 C 2 T x /Cd 0.8 Zn 0.2 S composites with Schottky junctions through the in-situ growth of Cd 0.8 Zn 0.2 S on Ti 3 C 2 T x nanosheets, enabling efficient photoreduction of U(VI) without the requirement of sacrificial agents. The results demonstrate that the Ti 3 C 2 T x /Cd 0.8 Zn 0.2 S composites achieve remarkable 99.48 % U(VI) reduction efficiency within 60 min in a 100 ppm uranium solution. Furthermore, the removal rate remains above 90 % after five cycles. The formation of Schottky heterojunctions by Ti 3 C 2 T x and Cd 0.8 Zn 0.2 S leads to the generation of an internal electric field that significantly promotes the rapid separation and transfer of photogenerated carriers, thereby enhancing the photocatalytic reduction efficiency of Ti 3 C 2 T x /Cd 0.8 Zn 0.2 S-3:100 (TC/CZS-3:100). A considerable amount of electrons accumulate on Ti 3 C 2 T x via the Schottky barrier, effectively facilitating the reduction of U(VI) to U(IV). As a co-catalyst, Ti 3 C 2 T x enhances the photocatalytic performance and stability of Cd 0.8 Zn 0.2 S. Moreover, the practical application in the waste liquid of rare earth tailings reveals that the removal rate can be as high as 91.24 %. This research is of significant value in the development of effective photocatalysts for the elimination of uranium from wastewater.

研究领域: 环境科学 · 材料科学
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JOURNAL OF MOLECULAR LIQUIDS · 2020 · IF 5.065

Unexpected ultrafast elimination of uranium and europium from aqueous solutions with magnetic bio-CaCO3

Huiyan Xiong,Jiemin Chen,Tingting Zhang,Wenzhong Wang,Chengcai Huang,Yuling Zhu,Baowei Hu

In this investigation, the magnetic bio-CaCO 3 were synthesized and elimination of uranium and europium from aqueous solutions. The prepared magnetic composite underwent a series of characterization analyses, such as Transmission electron microscope (TEM), Scanning electron microscopy-energy dispersive spectroscopy (SEM-EDS), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS), which prove that the magnetic particles are successfully modified on bio-CaCO 3. Surprisingly, it was found that coating the bio-CaCO 3 with Fe 3 O 4 not only increased the distance between the calcium carbonate nanosheets but also ensured the presence of Fe O active groups on the bio-CaCO 3 surface. The sorption of U(VI)/Eu(III) on the magnetic bio-CaCO 3 as a function of the pH, adsorbent dose, shaking time, co-existing ions, and the temperature was investigated using batch experiments. The effect of pH was investigated showing optimum sorption at pH 5 for U(VI) and Eu(III). The adsorption kinetics is relatively fast and can reach equilibrium in 60 to 90  min, and the pseudo-second-order rate equation preferentially fits the kinetic distribution, suggesting chemisorption was involved. The maximum adsorption amounts were 122.66 mg·g −1 for U(VI) and 130.62 mg·g −1 for Eu(III) at pH 5.0 and 298 K. The adsorption mechanism, which was evaluated with XRD, FTIR, SEM-EDS, and XPS, demonstrated that the functional groups (O H, -NH 2 , CO 3 2− and O Fe) and the increased hierarchical distances were primarily responsible for the improved adsorption ability. This paper highlights magnetic bio-CaCO 3 as potential, eco-friendly and ultrahigh-efficiency materials for uranium and europium pollution cleanup.

研究领域: 环境科学 · 材料科学
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2024 ·Vol. 333 ·期 3 ·1357-1365 · IF 1.5

Rapid radiochemical analysis of uranium and plutonium in emergency urine samples

Mei Lingzi,Shao Hui,Cui Lingzhi,Yang Jinmin,Zhang Lei

A novel method for rapid radioanalytical measurement of uranium and plutonium in 100ml emergency urine samples was developed, through optimized selection of the separation and purification process and a combined measurement with ICP-TOF-MS and alpha spectrometry. The typical analytical time is within 6 h, the recovery rates are more than 80%, and the minimum detection activity concentrations are 3.4 × 10 −4  Bq/L for 238 U and 2.5 × 10 −3  Bq/L for 239 Pu respectively. The spiked test shows that this method can be used for quantitative evaluation of the activity concentration of 238 U and 239 Pu in urine samples accurately.

研究领域: 放射化学 · 环境科学 · 医学检测
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2018 ·Vol. 317 ·期 3 ·1235-1241 · IF 1.181

Preparation of p-carboxyphenyl azo calix[4]arene phosphate derivative and its extraction properties toward uranium(VI)

Wang Cheng,Xiao Fang-zhu,Pu Yi-qiu,Xu Yu-li,Xu Dong-yang,Zhang Kang,Liu Yong,Peng Guo-wen

P -carboxyphenyl azo calix[4]arene phosphate derivative (P-CACPD) was successfully synthesized using calix[4]arene as raw material. The P-CACPD was characterized by FT-IR and 1 H-NMR. The effects of pH, extraction time and temperature on the extraction of U(VI) by P-CACPD were investigated. The results show that pH value, extraction time and temperature have an effect on the extraction of U(VI) by P-CACPD. When the initial pH is 5, temperature is 25 °C, extraction time is 2 h, the extraction rate of U(VI) by P-CACPD reaches the maximum. Both kinetics parameters and thermodynamic parameters of the extraction process were calculated. The calculated data indicate that the extraction process of uranium by P-CACPD is an exothermic spontaneous process, which well fits with the pseudo-second-order kinetic model.

CAS / MDL: 98-54-4
研究领域: 化学 · 环境科学
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CHEMOSPHERE · 2021 · IF 7.086

Insight into the performance and mechanism of persimmon tannin functionalized waste paper for U(VI) and Cr(VI) removal

Fenglei Liu,Shan Hua,Chao Wang,Baowei Hu

Herein, using dialdehyde waste paper (DAWP) as a cross-linking agent to immobilize persimmon tannin (PT) was first used to remove the U(VI) and Cr(VI) via the “waste control by waste” concept. The microscopic and macroscopic surface properties of the as-prepared adsorbent was characterized by the advanced characterization techniques. Factors that affected the elimination process such as variable pH, coexistence ions and equilibrium time were investigated by batch techniques. The results showed that the maximal removal capacities of U(VI) and Cr(VI) on DAWP-PT were 242.3 mg/g (pH = 6.0) and 178.7 mg/g (pH = 2.0) at 298 K, which exhibited competitiveness with most of the reported solid materials. Meanwhile, adsorption data were fitted perfectly to the Langmuir and Pseudo-second-order equations, which indicated that the monolayer and homogenous chemisorption dominated the removal process. The SEM-EDX, DFT and XPS analysis conformed that adsorption of U(VI) was mainly via surface complexation, while the elimination of Cr(VI) was a redox reaction process, and about 65.33% of Cr(III) and 34.67% of Cr(VI) co-existed onto the surface of DAWP-PT. Thus, this study would provide a high-efficiency and low-cost adsorbent for radionuclide and heavy metal treatment.

研究领域: 环境科学 · 材料科学
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Journal of Cleaner Production · 2023 · IF 11.1

Immobilization of uranium by S-NZVI and UiO-66-NO2 composite through combined adsorption and reduction

Di Zhang,Hao Tang,Bing Zhao,Lijie Liu,Hongwei Pang,Xiangxue Wang,Shujun Yu

Radioactive uranium removal plays a key role in energy development and environmental security. Sulfide nanoscale zero-valent iron (S-NZVI) has good antioxidant capacity, dispersibility and activity to eliminate U(VI) from wastewater, but the removal efficiency is limited. To improve the reduction and adsorption capacity of S-NZVI, through treating Fe 3+ solution by nitro-functionalized UiO-66 (UiO-66-NO 2 ) with high porosity, UiO-66-NO 2 enhanced S-NZVI adsorbent (S-NZVI/UiO-66) was prepared by liquid phase reduction method. The smaller size and larger specific surface area of S-NZVI/UiO-66 were confirmed by a variety of characterization techniques. Based on the excellent surface structure and reactivity, the U(VI) removal capacity of S-NZVI/UiO-66 (895 mg g −1 ) was much better than S-NZVI (434 mg g −1 ) and UiO-66-NO 2 (267 mg g −1 ). The impacts of pH, background ion strength, coexisting ions and different water environments on adsorption were studied via macroscopic batch experiments. The results showed that S-NZVI/UiO-66 could remove U(VI) adequately in a wide pH range. The removal rate was basically not affected by the concentration of NaNO 3 , demonstrating that the adsorption process of U(VI) on S-NZVI/UiO-66 tended to inner surface complexation. From XPS technique combined with the results of batch adsorption experiments, it was clear that the elimination mechanisms of U(VI) by S-NZVI/UiO-66 were mainly the physical adsorption, electrostatic attraction and complexation of UiO-66-NO 2 , and the reduction and complexation of S-NZVI. Therefore, it is believed that S-NZVI/UiO-66 has a great potential to be an excellent adsorbent in the field of the environment remediation. Moreover, S-NZVI/UiO-66 promises to be a novel nanomaterial for solving the problem of radionuclide contamination in practical environments.

研究领域: 环境科学 · 材料科学
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2014 ·Vol. 299 ·期 3 ·1911-1919 · IF 1.415

A label-free electrochemical biosensor for trace uranium based on DNAzymes and gold nanoparticles

Ma Dandan,Yuan Yali,Xiao Xilin,Gao Yangyang,Li Yuhui,Xu Wenhui,Long Wei

A novel and highly sensitive electrochemical DNAzymes biosensor was fabricated using Au nanoparticles (AuNPs) immobilized on the surface of Au electrode that had been previously modified with self-assembled monolayers of 1,6-hexanedithiol. Different modified electrodes were prepared and characterized by cyclic voltammetry and electrochemical impedance spectroscopy. The AuNPs were found to have a large surface area to anchor a large number of negatively charged phosphate backbones of DNAzymes, which further absorbed the electroactive indicator of hexaammineruthenium(III) ([Ru(NH 3 ) 6 ] 3+ ) to amplify the electrochemical signal. In the presence of target molecules, a large amount of DNA partly associated with [Ru(NH 3 ) 6 ] 3+ were removed from the electrode surface, leading to a significant decrease in peak current. Differential pulse voltammetry signals of [Ru(NH 3 ) 6 ] 3+ provided quantitative measures of the concentrations of uranyl ion (UO 2 2+ ), with linear calibration ranging from 13 pM to 0.15 nM and a detection limit of 5 pM. The presence of other metal ions did not affect the detection of UO 2 2+ , which indicated the high specificity of UO 2 2+ . Therefore, a new electrochemical DNAzymes sensor was designed with specific DNAzymes and AuNPs as immobilization platform and signal amplifier.

研究领域: 分析化学 · 环境科学 · 纳米技术 · 生物化学
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MOLECULES · 2024 ·Vol. 29 ·期 23 ·5759 · IF 4.2

Preparation and Evaluation of a Combination of Chelating Agents for the Removal of Inhaled Uranium

Lintao Li,Runtian Li,Ruohan Guo,Shuang Guo,Xuan Qiao,Xinru Wu,Peng Han,Yunbo Sun,Xiaoxia Zhu,Zhuona Wu,Hui Gan,Zhiyun Meng,Guifang Dou,Ruolan Gu,Shuchen Liu

Inhalation of aerosolized uranium is recognized as a principal mode of exposure, posing significant risks of damage to the lungs, kidneys, and other vital organs. To enhance nuclide elimination from the body, chelating agents are employed; however, single-component chelators often exhibit limited spectral activity and low effectiveness, resulting in toxicologically relevant concentrations. We have developed a composite chelating agent composed of 3,4,3-Li(1,2-HOPO), DFP, and HEDP in optimized ratios, demonstrating marked improvements in eliminating inhaled uranium. The selection of these components was initially guided by an agarose gel dynamics method, focusing on uranium binding and removal efficacy. Optimization of the formula was conducted through response surface methodology in a cellular model. The compound’s ability to enhance survival rates in mice subjected to acute uranium inhalation was confirmed, showing a dose-dependent improvement in survival in severely affected mice. Comparative assessments indicated that this multifaceted chelating agent substantially surpasses the uranium tissue clearance achieved by individual chelating agents.

CAS / MDL: 30652-11-0
研究领域: 毒理学 · 药理学 · 核医学 · 环境健康
✓ 已验证 产品关联 DOI PubMed 高影响因子
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JOURNAL OF HAZARDOUS MATERIALS · 2020 · IF 9.038

Highly efficient adsorption and immobilization of U(VI) from aqueous solution by alkalized MXene-supported nanoscale zero-valent iron

Siyi Wang,Lin Wang,Zijie Li,Pengcheng Zhang,Ke Du,Liyong Yuan,Shunyan Ning,Yuezhou Wei,Weiqun Shi

A novel composite of zero-valent iron nanoparticles supported on alkalized Ti 3 C 2 T x nanoflakes (nZVI/Alk-Ti 3 C 2 T x ) was constructed by an in-situ growth method for simultaneous adsorption and reduction U(VI) from aqueous solution in anoxic conditions . The effect of various factors such as adsorbent dose, pH, ionic strength, contact time, initial U(VI) concentration and environmental media were comprehensively investigated by batch experiments. Benefiting from the good dispersion uniformity of nZVI on MXene substrates, nZVI/Alk-Ti 3 C 2 T x exhibited rapid removal kinetics, excellent selectivity , 100% removal efficiency and up to 1315 mg g −1 uptake capacity for U(VI) capture. In the presence of mimic groundwater, 1.0 mM NaHCO 3 and 10 mg L −1 humic acid , the removal percentages of U(VI) by the composites could reach 95.1%, 88.9% and 69.5%, respectively. The reaction mechanism between U(VI) and nZVI/Alk-Ti 3 C 2 T x has been clarified based on FTIR , XANES , XPS and XRD analysis. Depending on the consumption of reactive nZVI in the composites and the solution pH, the elimination of U(VI) could be realized by different pathways including reductive immobilization in the form of UO 2 , inner-sphere surface complexation and hydrolysis precipitation. The present study illustrates that the nZVI/Alk-Ti 3 C 2 T x composite may be an efficient scavenger for radioactive wastewater purification in environmental remediation.

研究领域: 环境科学 · 材料科学
✓ 已验证 DOI PubMed 高影响因子
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ANALYTICA CHIMICA ACTA · 2024 · IF 5.7

Fluorescent Eu-MOF@nanocellulose-based nanopaper for rapid and sensitive detection of uranium (Ⅵ)

Yuqing Deng,Shan Jiang,Zifei Yan,Youlu Chu,Weibing Wu,Huining Xiao

Radioactive uranium leaks into natural water bodies mainly in the form of uranyl ions (UO 2 2+ ), posing ecological and human health risks. Fluorescent europium-based metal-organic frameworks (Eu-MOFs) have been demonstrated to be effective fluorescent sensors for UO 2 2+ , but the large size, powder state and poor dispersity limit their further application. In this work, fluorescent Eu-MOFs were in-situ grown on TEMPO-oxidized cellulose nanofibers (TOCNFs), which is the first time that spherical Eu-MOF crystals with sizes below 10 nm were prepared. Fluorescence spectral analysis revealed a nine-fold increase in the fluorescence intensity of TOCNF@Eu-MOF compared to Eu-MOF. The nanocomposites achieved rapid and sensitive fluorescence quenching to UO 2 2+ through the “antenna effect” and unsaturated Lewis basic sites on the ligands binding with UO 2 2+ . Moreover, TOCNF@Eu-MOF demonstrated excellent selectivity and anti-interference for UO 2 2+ detection. For the nanopaper-based sensor made from TOCNF@Eu-MOF, the Stern-Volmer quenching constant ( K SV ) was calculated as 8.21 × 10 4  M −1 , and the lowest limit of detection (LOD) was 6.6 × 10 −7  M, significantly lower than the 1.32 × 10 −6  M of Eu-MOFs. In addition, the nanopaper exhibited good fluorescence stability and cyclic detection performance, enabling the rapid and convenient detection of UO 2 2+ in the aqueous phase within 30 s by simple dipping.

CAS / MDL: 63557-10-8
研究领域: 材料科学 · 环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

Sub-Nano Gaδ+ clusters confined by porous carbon spheres and coupled with SnS2 for efficient photocatalytic extraction of uranium

Yuehua Pan,Yingxue Pang,Hao Fu,Zhenyu Cai,Yuxiang Deng,Zhiwei Huang,Donglou Ren,Yuezhou Wei,Xinpeng Wang

Extracting uranium from uranium waste streams, particularly utilizing zero-carbon emission photochemistry, emerges as a promising and sustainable strategy. Herein, we construct an SS@Ga/PCS composite photocatalyst, consisting of SnS 2 nanosheets as well as a metal − support produced by confining sub-nano Ga δ+ clusters in the hollow porous carbon spheres (PCS). The Ga δ+ clusters are innovatively introduced as active sites with localized hole capability to simultaneously improve visible light response and carrier separation. In-situ characterizations and theoretical calculations reveal that Ga δ+ clusters induced metal-support interaction (MSI) by optimizing the electronic structure in the PCS host; In addition, Ga δ+ clusters act as plasma excitation elements to enhance the visible light responsiveness and carrier separation of SS@Ga/PCS. Ultimately, the inhomogeneous photocatalysis of uranium extraction achieved superior performance as compared to the pure components, corresponding to an encouraging removal rate of 97.87 % and a photo-extraction capacity of up to 1867.30 mg g −1 in 50 mL of uranium waste solution, as well as a wide-concentration window adaptability and excellent catalytic robustness. More significantly, this ingenious nano-confined strategy extends the design ideas of highly dispersed sub-nanometallic cluster co-catalysts and stimulates the study of the availability of abundant reactive active sites combined with monomer strong interactions, which provides a novel insight into the mechanism of photocatalytic uranium extraction.

CAS / MDL: 69365-72-6
研究领域: 材料科学 · 环境科学 · 化学工程
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