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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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ACS Applied Materials & Interfaces · 2014 · IF 5.9

Adsorption-Induced Crystallization of U-Rich Nanocrystals on Nano-Mg(OH)2 and the Aqueous Uranyl Enrichment

Zhi Chen,Zanyong Zhuang,Qing Cao,Xiaohong Pan,Xiong Guan,Zhang Lin

The mechanism of the interaction between nano-Mg(OH)2 adsorbent and uranyl in water was studied. At trace levels, the uranyl is adsorbed as a monolayer on nano-Mg(OH)2, and occupied a small proportion of the adsorption sites. As the uranyl concentration crosses over a threshold, continuous increase of adsorption capacity takes place. It indicates that, by taking the pre-adsorbed uranyl as the nucleation centers, the additional uranyl crystallizes and forms U-rich nanocrystals well-scattered on the surface of nano-Mg(OH)2. A strategy of inducing fast crystal growth of nano-Mg(OH)2 to micrometer-sized Na2Mg(CO3)2 enables the desorption and enrichment of uranyl. The recycling and reuse of nano-Mg(OH)2 can be achieved simultaneously. The finding in this work provides fundamental understanding of the efficient usage of nano-Mg(OH)2 in practical applications.

研究领域: 材料科学 · 环境科学
✓ 已验证 DOI PubMed 高影响因子
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2017 ·Vol. 312 ·期 2 ·187-198 · IF 1.282

Adsorptive removal of uranyl ions in aqueous solution using hydrothermal carbon spheres functionalized with 4-aminoacetophenone oxime group

Zheng Zhiyang,Wang Youqun,Zhao Wuwei,Xiong Guoxuan,Cao Xiaohong,Dai Ying,Le Zhanggao,Yu Shenglong,Zhang Zhibin,Liu Yunhai

Hydrothermal carbon spheres (HCSs) functionalized with 4-aminoacetophenone oxime group (HCSs-oxime) were prepared by a grafting method and explored to adsorption of uranyl ions from aqueous solution. The results of FT-IR, elemental analysis and zeta potential indicate a successfully modification with oxime group. The adsorbent shows an excellent adsorption capacity (Langmuir, q m  = 588.2 mg g −1 ) and quick adsorption kinetic (equilibrium time of approximately 60 min) at optimal pH of 6.0. The adsorptive selectivity for uranyl ions has been also great improved in present with various co-existing ions. Overall, HCSs-oxime is a potentially promising material for selective removal of uranium in the contaminated solution.

研究领域: 环境科学 · 材料科学 · 核化学 · 水污染治理 · 功能材料
✓ 已验证 DOI 高影响因子
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MICROCHIMICA ACTA · 2015 ·Vol. 183 ·期 1 ·407-413 · IF 3.741

Arsenazo III-functionalized gold nanoparticles for photometric determination of uranyl ion

Liang Yun,He Yi

Gold nanoparticles (AuNPs) were functionalized with the indicator dye Arsenazo III via reductive synthesis of AuNPs in the presence of arsenazo III. The indicator dye is shown to be immobilized on the AuNPs via interaction between gold and sulfo groups. The functionalized AuNPs undergo aggregation in the presence of uranyl ion due to the coordination interaction between arsenazo III and uranyl ion. This is accompanied by a longwave shift of the surface plasmon resonance absorption band (from 535 nm to 548 nm) and an up to 46.8 % increase in absorbance. This finding forms the basis for a photometric assay for uranyl ion. It shows good selectivity and has a 0.5 μM detection limit. Applied to the determination of uranyl ion in spiked environmental water samples, the recoveries were between 97 and 106 %. Arsenazo III dye functionalized gold nanoparticles (AuNPs) were prepared via a one-pot reduction reaction. Based on the coordination interaction of arsenazo III functionalized AuNPs and uranyl ion, an assay for uranyl ion was developed.

研究领域: 分析化学 · 环境科学
✓ 已验证 DOI 高影响因子
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CHEMICAL PAPERS · 2020 ·Vol. 74 ·期 7 ·2049-2057 · IF 1.68

Extraction and separation of thorium(IV) and uranium(VI) with 4-oxaheptanediamide into ionic liquid system from aqueous solution

Ren Peng,Li Yang,Wang Zhifen,Geng Yanxia,Yu Tao,Hua Rong

Thorium is much more abundant than uranium in nature and has become one of the important potential energy sources in the future. It is because that a thorium-232( 232 Th) nucleus has the ability to produce a uranium-233( 233 U) nucleus by absorbing a neutron. The aim of this paper is to investigate the extraction and separation of thorium ions and uranyl ions from aqueous solution with N,N’ -dimethyl- N,N’ -dioctyl-4-oxaheptanediamide (DMDOHA) into ionic liquids of 1-methyl-3-butylimid-azolium bis(trifluoromethanesulfonyl)imide ([C 4 mim][NTf 2 ]). The results show that the extractant DMDOHA has a good affinity toward thorium ions than uranyl ions in the present system, the maximum value of separation factor SF Th(IV)/U(VI) is 21.9 at pH 2.24. The extraction process of thorium ions and uranyl ions was confirmed to proceed by cation-exchange extraction mechanism. The DMDOHA extractant formed a major 3:1 complex with thorium ion and a major 2:1 complex with uranyl ion based on the relationship between log[DMDOHA] with logD.

研究领域: 化学 · 核能科学
✓ 已验证 DOI 高影响因子
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NEW JOURNAL OF CHEMISTRY · 2023 ·Vol. 47 ·期 10 ·4667-4673 · IF 3.3

Smartphone-assisted colorimetric determination of uranyl ions in aqueous solutions

Yufei Lei,Yujie Li,Chen Liu,Liqiong He,Qian Li,Lifu Liao,Xilin Xiao

A convenient and portable smartphone-assisted method for the colorimetric detection of uranyl ions (UO22+) in aqueous solutions is proposed using rifampicin and 2-(5-bromo-2-pyridylazo)-5-diethylaminophenol (Br-PADAP) as chromogenic agents. The addition of UO22+ would cause reaction with chromogenic agents to form complexes, changing the colour from orange to dark red in the rifampicin system and from yellow to light pink in the Br-PADAP system. To achieve the on-site estimation of the trace UO22+ concentration range, digital images of colour changes captured by the smartphone under fixed lighting conditions were imported into the built-in application named “Detect” to obtain HSV (hue, saturation, and value) and HSL (hue, saturation, lightness) information, which could be associated with the concentration of uranyl ions. For more precise laboratory-level detection, ultraviolet-visible (UV-vis) spectroscopy was employed as well. The absorbance of the rifampicin system exhibited strong linearity with the UO22+ concentration in the range from 4 to 50 μM at 375 nm with a method detection limit (MDL) of 3.17 μM by the UV-vis-based method, while that of Br-PADAP system had a linear relationship with the concentration from 0.9 to 7 μM at 562 nm with an MDL of 0.89 μM. The two strategies may be combined to detect UO22+ across a larger concentration range, and this method has been successfully used to analyze real samples including soil around uranium mines.

研究领域: 分析化学 · 环境科学
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BIOSENSORS & BIOELECTRONICS · 2022 · IF 12.545

Smart DNA-gold nanoparticle hybrid hydrogel film based portable, cost-effective and storable biosensing system for the colorimetric detection of lead (II) and uranyl ions

Chang Liu,Siyu Gou,Yanhui Bi,Qi Gao,Juanjuan Sun,Shanjin Hu,Weiwei Guo

A portable, cost-effective and storable DNA-gold nanoparticle (AuNP) hybrid hydrogel film based biosensing system was developed, with AuNPs serving as both the crosslinking units of the film and the signaling units. Using a layer-by-layer assembly method, hydrogel film composed of three-dimensional hydrophilic network of densely packed AuNPs interconnected by responsive DNA structures was constructed onto a glass slide. By programming the sequence of DNA structures, target-responsive hybrid films were constructed. As a proof of concept , the sequence of a substrate DNA which can be identified and cleaved by Pb 2+ -dependent DNAzyme was encoded to construct Pb 2+ -responsive DNA-AuNP hybrid hydrogel film. The high-density packing of AuNPs as signal substances significantly improved the sensitivity of the ultrathin film biosensing system while reduced the cost of expensive DNA materials. A hydrogel film composed of 10 layers of assembled DNA-AuNP structures generated sufficient visual colorimetric signals for Pb 2+ detection, with a detection limit of 2.6 nM. By introducing UO 2 2+ -dependent DNAzyme, the system could be further applied in the sensitive and selective detection of UO 2 2+ , with a detection limit of 10.3 nM. Compared with bulk-sized DNA hydrogel biosensing systems, the DNA-AuNP hydrogel film biosensing system exhibited faster response thanks to the sub-micrometer ultrathin film structures. Moreover, the protection of fragile non-covalently crosslinked DNA films with solid slides also facilitated the portable application and long-term storage of the resulting biosensing system, with 95% of the response signal retained after three months of storage. The DNA-AuNPs hydrogel film biosensing system is highly promising for future rapid on-site detection applications.

研究领域: 生物化学 · 纳米生物学 · 环境科学
✓ 已验证 DOI 高影响因子
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INORGANIC CHEMISTRY · 2017 · IF 4.857

Exploring New Assembly Modes of Uranyl Terephthalate: Templated Syntheses and Structural Regulation of a Series of Rare 2D → 3D Polycatenated Frameworks

Lei Mei,Cong-zhi Wang,Liu-zheng Zhu,Zeng-qiang Gao,Zhi-fang Chai,John K. Gibson,Wei-qun Shi

The reaction of uranyl nitrate with terephthalic acid (H2TP) under hydrothermal conditions in the presence of an organic base, 1,3-(4,4′-bispyridyl)propane (BPP) or 4,4′-bipyridine (BPY), provided four uranyl terephthalate compounds with different entangled structures by a pH-tuning method. [UO2(TP)1.5](H2BPP)0.5·2H2O (1) obtained in a relatively acidic solution (final aqueous pH, 4.28) crystallizes in the form of a noninterpenetrated honeycomb-like two-dimensional network structure. An elevation of the solution pH (final pH, 5.21) promotes the formation of a dimeric uranyl-mediated polycatenated framework, [(UO2)2(μ-OH)2(TP)2]2(H2BPP)2·4.5H2O (2). Another new polycatenated framework with a monomeric uranyl unit, [(UO2)2(TP)3](H2BPP) (3), begins to emerge as a minor accompanying product of 2 when the pH is increased up to 6.61, and turns out to be a significant product at pH 7.00. When more rigid but small-size BPY molecules replace BPP molecules, [UO2(TP)1.5](H2BPP)0.5 (4) with a polycatenated framework similar to 3 was obtained in a relatively acidic solution (final pH, 4.81). The successful preparation of 2–4 represents the first report of uranyl–organic polycatenated frameworks derived from a simple H2TP linker. A direct comparison between these polycatenated frameworks and previously reported uranyl terephthalate compounds suggests that the template and cavity-filling effects of organic bases (such as BPP or BPY), in combination with specific hydrothermal conditions, promote the formation of uranyl terephthalate polycatenated frameworks.

研究领域: 化学 · 材料科学
✓ 已验证 DOI 高影响因子
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Journal of Environmental Sciences · 2018 · IF 3.12

Sorption of uranyl ions on TiO2: Effects of pH, contact time, ionic strength, temperature and HA

Jingjing Wang,Bihong He,Xiaoyan Wei,Ping Li,Jianjun Liang,Shirong Qiang,Qiaohui Fan,Wangsuo Wu

Sorption of U(VI) onto TiO 2 as functions of pH, ionic strength, contact time, soil humic acid (SHA), solid-to-liquid ratio and temperature was studied under ambient conditions using batch and spectroscopic approaches. The sorption of U(VI) on TiO 2 was significantly dependent on pH and ionic strength. The presence of SHA slightly enhanced the sorption of U(VI) on TiO 2 below pH   4.0, while it inhibited U(VI) sorption in the higher pH range. U(VI) sorption on TiO 2 was favored at high temperatures, and the sorption process was estimated to be endothermic and spontaneous. Reduction of U(VI) to lower valent species was confirmed by X-ray photo-electron spectroscopy analysis. It is very interesting to find that U(VI) sorption on TiO 2 was promoted in solutions with higher back-ground electrolyte concentrations. In the presence of U(VI), higher back-ground electrolyte made more TiO 2 particles aggregate through (001) facets, leading more (101) facets to be exposed. Therefore, the reduction of U(VI) was enhanced by the exposed (101) facets and more U(VI) removal was observed.

CAS / MDL: 13463-67-7
研究领域: 环境科学 · 化学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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BIOSENSORS & BIOELECTRONICS · 2015 · IF 6.409

Magnetic beads-based DNAzyme recognition and AuNPs-based enzymatic catalysis amplification for visual detection of trace uranyl ion in aqueous environment

Hongyan Zhang,Ling Lin,Xiaoxue Zeng,Yajuan Ruan,Yongning Wu,Minggui Lin,Ye He,FengFu Fu

We herein developed a novel biosensor for the visual detection of trace uranyl ion ( UO 2 2 + ) in aqueous environment with high sensitivity and specificity by using DNAzyme-functionalized magnetic beads (MBs) for UO 2 2 + recognition and gold nano-particles (AuNPs)-based enzymatic catalysis oxidation of TMB (3,3′,5,5′-tetramethylbenzidine sulfate) for signal generation. The utilization of MBs facilitates the magnetic separation and collection of sensing system from complex sample solution, which leads to more convenient experimental operation and more strong resistibility of the biosensor to the matrix of sample, and the utilization of AuNPs-based enzymatic catalysis amplification greatly improved the sensitivity of the biosensor. Compared with the previous DNAzyme-based UO 2 2 + sensors, the proposed biosensor has outstanding advantages such as relative high sensitivity and specificity, operation convenience, low cost and more strong resistibility to the matrix of sample. It can be used to detect as low as 0.02   ppb (74   pM) of UO 2 2 + in aqueous environment by only naked-eye observation and 1.89   ppt (7.0   pM) of UO 2 2 + by UV–visible spectrophotometer with a recovery of 93–99% and a RSD≤5.0% ( n =6) within 3   h. Especially, the visual detection limit of 0.02   ppb (74   pM) is much lower than the maximum allowable level of UO 2 2 + (130   nM) in the drinking water defined by the U.S. Environmental Protection Agency (EPA), indicating that our method meets the requirement of rapid and on-site detection of UO 2 2 + in the aqueous environment by only naked-eye observation.

CAS / MDL: 16961-25-4 68-04-2
研究领域: 环境科学 · 生物传感 · 纳米技术
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SCIENCE OF THE TOTAL ENVIRONMENT · 2022 · IF 10.753

Valence regulation investigation of key factors on the electrochemical immobilization uranyl from wastewater

Jianzhang Gao,Jiadong Wang,Jiaqi Chen,Shitao Liao,Meng Cao,Fuqiu Ma,Yun Xue,Yongde Yan

Electrochemical techniques are considered promising applications to immobilize uranium in alkaline wastewater in order to prevent its migration into groundwater and soil. In this work, the results of electrochemical and Atomic Force Microscope (AFM) demonstrate a successful immobilization of uranyl in the carbonate system by U(VI)-U(V), U(V)-U(IV) reduction, and U(V) disproportionation reactions. The results indicated that the electrochemical fixation rate in alkaline system could reach more than 99%. The valence state of uranium is the key factor affecting its migration in the working system. Where, the analysis of the immobilized samples by X-ray photoelectron spectroscopy (XPS) revealed that pHs, current density, and the presence of foreign cations significantly affect the valence state of uranium in the immobilized samples. Under same conditions, the reduction reactions of U(VI)-U(V) and U(V)-U(IV) occurred easily. Where, at pH higher than 3.4 or the current density in the range of 0.5–20 mA/cm 2 , high content of U(V) and U(IV) in the immobilized products was obtained. Other conditions favored the occurrence of the electrolytic water reaction, and the immobilized samples were dominated by U(VI). It was found that the temperature showed the greatest effect on the electrochemical immobilization rate. Where, the electrochemical immobilization rate increased by about 1.8 times when the ambient temperature increased from 293.15 to 328.15 K. This study provides a new idea for the immobilization of uranium in alkaline wastewater and demonstrates the feasibility of electrochemical immobilization of uranium in alkaline systems.

研究领域: 环境科学 · 电化学工程
✓ 已验证 产品关联 DOI PubMed 高影响因子
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2024 · IF 1.5

Development of rare earth europium composites for highly sensitive fluorescence enhancement for detection of uranyl ions in water and cells

Zhou Xiayu,Wang Yue,Xiong Lihao,Song Jiayi,Zhou Huang,Li Le,Zhen Deshuai

Uranium plays a crucial role in the nuclear energy sector, yet its radiological and chemical characteristics can pose environmental and public health hazards. This study introduces a novel bimetallic system based on cation-cation interactions, involving the binding of europium ions (Eu 3+ ) to uranyl ions (UO 2 2+ ) via phosphate bridges. The method exhibits excellent linearity in the uranyl ion concentration range of 10–90 nM, with a detection limit as low as 10 nM. The system has been successfully applied to detect UO 2 2+ in actual water samples and for fluorescence imaging of UO 2 2+ in cells. These findings highlight the potential of Eu-P as a promising material for sensing UO 2 2+ , offering significant contributions to environmental monitoring and public health protection.

CAS / MDL: 7647-14-5
研究领域: 环境科学 · 分析化学 · 生物医学
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