ACS Applied Polymer Materials
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2025
·
IF 4.7
Shaobo Ren,Zhiming Li,Ju Lv,Pengfei Han,Xinyue Zhang,Lang Pan,Ying You,Xueqiong Yin,Xingqing Xiao
The ion imprinting technique was applied in this work to prepare a thermosensitive biomass-based polymeric hydrogel, termed UITB, which exhibits unique temperature-dependent swelling behavior: it shrinks at high temperatures but swells at low temperatures. The reversible swelling property enables the UITB polymer gel to capture and release UO22+ ions by adjusting the temperature within a moderate range of 20°C–45°C. A high adsorption selectivity of UITB for the target UO22+ ions was observed in the presence of decoy metal ions. Rinsing with pure water for the elution of the absorbed UO22+ greatly extends the lifetime of the polymer gel. Subsequently, various thermodynamic models were used to theoretically study the adsorption equilibrium and kinetics of UITB. A monolayer adsorption was identified, with the adsorption dynamics being controlled by both the diffusion process and electron transfer. To explore the molecular mechanism of UO22+ adsorption at the microscale level, atomistic molecular dynamics simulations were performed to investigate the adsorption behavior of UO22+ in two computationally modeled hydrogel network units of different pore sizes. Analysis of the energies showed that the negative intermolecular ELE+EGB energy is responsible for the adsorption and desorption of UO22+ on the polymer gel, while the positive intermolecular VDW energy indicates that the UO22+ ions are prevented from being absorbed anywhere except within the cavities. Finally, testing of the application revealed that our UITB polymer gel demonstrates effective adsorption capabilities for UO22+ in natural seawater, highlighting its potential for practical use.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
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2025
·Vol. 39
·期 6
·e70213
·
IF 0
Zhi-Zhou Chen,Shuo Wang,Wen-Jie Jiang,Zhi-Hao Cai,Chen-Hao Zhang,Ming-Yu Huang,Guang-Zao Huang,Dan Zhao
Uranium can cause irreversible reactions in the body if accidentally ingested by organisms, and when antibiotics exceed normal acceptable levels, they can cause serious illness, so detecting them is important but also challenging. In this work, new azo-imidazole ligands were formed by introducing different functional groups (biphenol, phenol) into the benzimidazole moiety (E)-4-((1H-benzo[d]imidazol-5-yl)diazenyl)-[1,1′-biphenyl]-2,2′-diol [L1]、(E)-3-((1H-benzo[d]imidazol-5-yl)diazenyl)phenol [L2]. Subsequently, under different high temperature, a series of water-stabilized Zn-based metal–organic frameworks (MOFs) [Zn(L1)(BDC)]·CH 3 OH·H 2 O ( MOF-1 ), [Zn 2 (L2) 4 (BDC) 2 ]·L2 ( MOF-2 ) and [Zn(L2)(1,3-BDC)]·H 2 O ( MOF-3 ) were obtained by using H 2 BDC and 1,3-H 2 BDC as auxiliary ligands. X-ray revealed that they were different 3D supramolecular framework. Outstanding fluorescent properties and structural stability of MOFs 1-3 making them potential luminescent sensors for UO 2 2+ ions and antibiotics in water. The results show that MOF-1 , MOF-2 , and MOF-3 exhibit high sensitivity for the detection of UO 2 2+ ions with detection limits of 3.00 × 10 −6 mol/L for MOF-1 , 2.58 × 10 −6 mol/L for MOF-2 , and 3.01 × 10 −6 mol/L for MOF-3 . Similarly, the strong emissions of MOF-1 , MOF-2 , and MOF-3 can be quenched efficiently by trace amount of NMs (metronidazole, MDZ; dimetridazole, DTZ) and NFs antibiotics (nitrofurazone, NZF; nitrofurantoin, NFT; furazolidone, FZD).
研究领域:
材料科学
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环境科学
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化学
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DOI
MICROPOROUS AND MESOPOROUS MATERIALS
·
2020
·
IF 4.551
Yaorui Li,Adede Ochieng Simon,Caishan Jiao,Meng Zhang,Wenfu Yan,Heng Rao,Jiancong Liu,Jianan Zhang
In this study, a new and efficient sorbent material was developed by the surface modification of zeolite Y with surfactant of cetyltrimethyl ammonium bromide (CTAB) and amino acid of l -aspartic acid (Asp) for rapid removal of Sr 2+ , Cs + and UO 2 2+ in solution. The as-synthesized and modified zeolite Y were characterized by powder X-ray diffraction (XRD), scanning electron microscope (SEM), thermogravimetric analysis (TGA), Fourier transform infrared spectroscopy (FTIR) and nitrogen adsorption-desorption analysis. The results showed that after first grafting the cations of CTAB on the external surface of zeolite Y crystals, negatively charged Asp was then successfully introduced onto zeolite to form the CTAB + Asp dually modified zeolite Y sorbent . The fraction of CTAB and Asp in dually modified zeolite Y is 9.6 wt % and 16.3 wt %, respectively. The sorption isotherm of UO 2 2+ , Sr 2+ and Cs + by such sorbent was better fitted by Langmuir model. The CTAB + Asp dually modified zeolite Y took 20 min to reach the maximum sorption amount, while the unmodified zeolite Y took 240 min. This encouraging result provides a new concept to design sorbent materials for rapid removal of radionuclides from contaminated water system in an emergency.
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DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
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2022
·Vol. 331
·期 11
·4635-4648
·
IF 1.754
Liu Chang,Li Ye,Liu Shuang,Zhou Yuzhi,Liu Dongxue,Fu Chengbin,Ye Lingfeng
In this work, an inexpensive PEI-AC sorbent was synthesized by facile hydrothermal grafting method and used to uranium capture from seawater. Batch experimental demonstrated that the optimal operation pH of PEI-AC was 6.0. The adsorption process is conformed to pseudo-second-order kinetic model and Langmuir monolayer adsorption isotherm, and the maximum equilibrium adsorption capacity reached 50.27 mg/g. The PEI-AC samples exhibited better selective and efficiency in various competing ions and uranium-spiked seawater. Furthermore, the removal efficiency remained 88.52% after five sequence adsorption/desorption experiments. By the analysis of XPS, the interaction of UO 2 2+ with N/O-containing ligands were the primary immobilization mechanism.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
BIOSENSORS & BIOELECTRONICS
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2025
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IF 10.5
Deshuai Zhen,Qiuhui Deng,Yao Yu,Sihan Chen,Le Li,Qingyun Cai,Yu Liu
A highly sensitive, selective, and simple method for detecting uranyl ions (UO 2 2+ ) is crucial for human health and environmental safety. Amidoxime-based nanomaterials have been widely employed for UO 2 2+ detection, but their higher affinity for vanadium than UO 2 2+ limits their practical applications. Herein, a novel covalent organic polymer fluorescent probe (TT-COP) for UO 2 2+ detection was innovatively developed by a one-step Schiff-base condensation reaction between 3,3′,5,5′-tetramethylbenzidine (TMB) and 2,4,6-triformylphloroglucinol (Tp). TT-COP not only possesses excellent thermodynamic stability, hydrophilicity, synthetic reproducibility, and fluorescence stability but also achieves outstanding sensing performance, with its interaction with UO 2 2+ reaching equilibrium within 5 min and a detection limit of 35.75 nM. Further investigations reveal that UO 2 2+ coordinates with the imine and hydroxyl groups of TT-COP, thereby inhibiting the intramolecular charge transfer (ICT) process and leading to fluorescence quenching. Moreover, TT-COP exhibits extraordinary selectivity and biocompatibility, enabling reliable UO 2 2+ quantification in complex matrices including environmental waters, food, and biological samples, with recovery rates ranging from 94.54 % to 106.43 %. The detection results closely align with those obtained from high-precision ICP-MS measurements. These findings underscore the promising practical applications of TT-COP in food safety, environmental monitoring, and human health assessment.
研究领域:
分析化学
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环境科学
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材料科学
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食品安全
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生物化学
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DOI
PubMed
高影响因子
Journal of Environmental Sciences
·
2026
·
IF 6.5
Mingcai Ma,Bin Mu,Jiang Xu,Yushen Lu,Aiqin Wang
With the increasingly serious problems of resource depletion and environmental pollution, it has become a key path to synthesize low-cost and high-value-added functional materials through recycling waste resources. Inspired by the sustainable development concept of "turning waste into treasure", two bimetallic metal-organic frameworks (BMOFs) of MIL-53(Al, Fe) and NH 2 -MIL-53(Al, Fe) were successfully prepared by a one-pot hydrothermal method using acid-leaching wastewater generated from the whitening process of mixed-dimensional attapulgite clay as the metal ion source and reaction medium. The obtained BMOFs presented excellent crystallinity, acid-base stability, and adsorption performance for Pb 2+ (263.2 and 304.0 mg/g) and UO 2 2+ (497.5 and 704.2 mg/g). The involved adsorption mechanisms were mainly attributed to coordination and electrostatic interactions. This research realized the sustainable utilization of acid-leaching wastewater during fine-processing of non-metallic minerals, and significantly reduced the synthesis cost of MOFs, embodying the sustainable development goal of 3Rs (reduce, reuse and recycle) concept.
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高影响因子
MICROCHIMICA ACTA
·
2020
·Vol. 187
·期 5
·1-9
·
IF 6.232
Cao Chen,Liu Jinquan,Tang Shuangyang,Dai Zhongran,Xiao Fubing,Rang Weiqing,Liu Ling,Chen Tuo,Yuan Yali,Li Le
A superior electrochemical biosensor was designed for the determination of UO 2 2+ in aqueous solution by integration of DNAzyme and DNA-modified gold nanoparticle (DNA-AuNP) network structure. Key features of this method include UO 2 2+ inducing the cleavage of the DNAzyme and signal amplification of DNA-AuNP network structure. In this electrochemical method, the DNA-AuNP network structure can be effectively modified on the surface of gold electrode and then employed as an ideal signal amplification unit to generate amplified electrochemical response by inserting a large amount of electrochemically active indicator methylene blue (MB). In the presence of UO 2 2+ , the specific sites on DNA-AuNP network structure can be cleaved by UO 2 2+ , releasing the DNA-AuNP network structure with detectable reduction of electrochemical response intensity. The electrochemical response intensity is related to the concentration of UO 2 2+ . The logarithm of electrochemical response intensity and UO 2 2+ concentration showed a wide linear range of 10~100 pM, and the detection limit reached 8.1 pM (S/ N = 3). This method is successfully used for determination of UO 2 2+ in water samples.
Fabricated DNAzyme network structure for enhanced electrical signal. Numerical experiments show that the current signal decreases as the concentration of UO 2 2+ increases. It can be seen that the biosensors could be used to detect UO 2 2+ in aqueous solution effectively.
研究领域:
生物化学
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环境科学
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分析化学
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DOI
PubMed
高影响因子
MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Wen-Juan Gong,Hua-Rui Nan,Hong-Bo Peng,You-Qun Wang,Zhi-Min Dong,Zhi-Bin Zhang,Xiao-Hong Cao,Yun-Hai Liu
In this study, we prepared a new ratiometric fluorescent sensor by first encapsulating blue-fluorescent carbon dots (B-CDs) with SiO 2 , coupling gold nanoclusters (GSH-AuNCs) to the surface, and finally anchoring a layer of Ag + . The presence of UO 2 2+ caused fluorescence quenching of the ratiometric fluorescent probe when used in aqueous solutions. Furthermore, HOMO–LUMO orbital analysis suggested that the quenching mechanism was mainly attributed to photoinduced electron transfer (PET) between B-CDs@SiO 2 @GSH-AuNCs/Ag + and UO 2 2+ . Under optimal conditions, the ratiometric fluorescent probes exhibited excellent selectivity and detected UO 2 2+ at 37 nmol/L. This new “on–off” ratiometric fluorescent sensor exhibits promising potential for convenient monitoring of UO 2 2+ levels with ideal recovery in real-world water samples.
研究领域:
分析化学
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环境科学
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材料科学
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DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2023
·
IF 6
Qiqi Guo,Yizhi Chen,Peng Zhang,Yusen Liu,Yifan Li,Yu Yang,Qi Cao,Mingzhang Lin
In the present work, the effects of four neutral phosphorus extractants (TBP, TAP, THP, TEHP) with different molecular structures on the extraction behaviors towards U(Ⅵ) and radiation stability were systematically studied. The results of the batch extraction and the γ-radiolysis experiments manifested that the extraction performance and radiation stability of the four extractants followed the order of TEHP > THP > TAP > TBP. Moreover, DFT calculations and Multiwfn software were utilized to analyze the properties of the extractants. The electrostatic potentials (ESP) and frontier molecular orbital of extractants indicated that the nucleophilic ability was ranked as TEHP > THP > TAP > TBP. The analyses of quantum theory of atoms in molecules (QTAIM) and Wiberg indices (WBIs) revealed that the UO 2 2+ ions exhibited stronger complexation ability with O atoms in TEHP compared to the other three extractants. The bonds between UO 2 2+ ions and extractants were primarily ionic in nature. From the energetic perspective, the thermodynamic energy demonstrated that the Gibbs free energy of TEHP in aqueous solution was the most negative, implying that it should be easier to combine with UO 2 2+ . This work elucidates that the increase of alkyl chain length and the presence of branched chains can enhance the extraction performance and radiation stability of neutral phosphorus extractants. It not only lays the theoretical foundation for designing novel organic phosphorous extractants with superior extraction performance and high radiation stability, but also provides scientific basis for the extraction process of uranium in spent nuclear fuel reprocessing.
研究领域:
化学工程
·
核化学与放射化学
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高影响因子
INORGANICA CHIMICA ACTA
·
2021
·
IF 2.545
Xingliang Li,Juncai Lu,Wanjun Mu,Baihua Chen,Daibing Luo,Bijun Liu,Yanqiu Yang,Hongyuan Wei,Shuming Peng
Nitrilotri–3–propanoic Acid (NTPA) and Tris(2–carboxyethyl) phosphine (TCEP) possess similar skeleton. This pair of isostructural ligands is a perfect set to assess the differences of uranyl (UO 2 2+ ) complexes with N–tricarboxylate versus P–tricarboxylate. The protonation reactions of NTPA and TCEP were investigated by potentiometry and calorimetry. Complexation of uranyl with the both ligands was studied by potentiometry and structural analysis. The results indicate that central trialkylamine in NTPA has a higher affinity for the proton than trialkylphosphine in TCEP. Crystal structures and NMR analyses indicate that central amine of NTPA and central phosphine of TCEP are not involved in the bonding. NTPA/UO 2 2+ complex is more stable than TCEP/UO 2 2+ complex. This difference cannot be explained by electronic effect of central N and P atoms because of nonbonding interactions. The higher stability of UO 2 2+ /NTPA versus UO 2 2+ /TCEP may be due to the fact that the central N atom of NTPA has a lower steric hindrance than the central P atom of TCEP. Another possible reason is that UO 2 2+ /TCEP complexes have different coordination modes from UO 2 2+ /NTPA complexes.
研究领域:
化学
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配位化学
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核化学
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DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Xin-Yu Wang,Yang Hao,Hong-Bo Zhao,Yuan-Ru Guo,Qing-Jiang Pan
The interfacial chemistry of nanocomposite materials is of overarching importance in the separation and purification science; moreover, its understanding helps to guide synthesis, clarify structure-property relationship and unearth novel applications. However, the composites feature rather complicated local structures and hydrogen bonds are often involved in the interface and the vicinity of active sites. In this regard, density functional theory first-principle calculations associated with experimental study have synergistically examined two-dimensional (2D) magnesium hydroxide material with different layers and their adsorption toward cellobiose. Hydrogen bonds are found responsible for the interfacial coupling, which make it vital to cover the dispersion correction in the calculation. The average adsorption energy ranges from −0.29 to −0.35 eV, falling well within the range of reported hydrogen-bonding strength. On the basis of calculated structural/interfacial properties and experimental findings, the 2D Mg(OH) 2 in terms of three-layer model was unraveled to substitute toxic Cd 2+ ion and sorb radioactive UO 2 2+ that is coordinated by water and hydroxyl groups. These reactions are thermodynamically feasible. The ion-exchanging mechanism was proposed for cadmium removal and the outer-sphere adsorption one for uranium extraction.
研究领域:
材料科学
·
环境科学
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产品关联
DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2024
·
IF 6.7
Junhua Chen,Xu Wang,Junhui Guo,Yiwen Lv,Manjia Chen,Hui Tong,Chengshuai Liu
The uranyl ion (UO22+) is the most stable form of uranium, which exhibits high toxicity and bioavailability posing a severe risk to human health. The construction of ultrasensitive, reliable, and robust sensing techniques for UO22+ detection in water and soil samples remains a challenge. Herein, a DNA network biosensor was fabricated for UO22+ detection using DNAzyme as the heavy metal recognition element and double-loop hairpin probes as DNA assembly materials. UO22+-activated specific cleavage of the DNAzyme will liberate the triggered DNA fragment, which can be utilized to launch a double-loop hairpin probe assembly among Hab, Hbc, and Hca. Through multiple cyclic cross-hybridization reactions, hexagonal DNA duplex nanostructures (n[Hab•Hbc•Hca]) were formed. This DNA network sensing system generates a high fluorescence response for UO22+ monitoring. The biosensor is ultrasensitive, with a detection limit of 2 pM. This sensing system also displays an excellent selectivity and robustness, enabling the DNA network biosensor to work even in complex water and soil samples with excellent accuracy and reliability. With the advantages of enzyme-free operation, outstanding specificity, and high sensitivity, our proposed DNA network biosensor provides a reliable, simple, and robust method for trace levels of UO22+ detection in environmental samples.
研究领域:
生物化学
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环境科学
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DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）