期刊：
Separation and Purification Technology,2025年354:129241 ISSN：1383-5866
通讯作者：
Zhongran Dai
作者机构：
[Dai, Zhongran; Liang, Beichao; Chen, Lijie] Key Discipline Laboratory for National Defense for Biotechnology in Uranium Mining and Hydrometallurgy, University of South China, Hengyang 421001, China;[Zhang, Weilin] College of Public Health, Hengyang Medical School, University of South China, Hengyang 421001, Hunan, China;[Gao, Yuan] School of Chemical Engineering and Technology, China University of Mining & Technology, Xuzhou, Jiangsu 221116, China;[Li, Le] Key Discipline Laboratory for National Defense for Biotechnology in Uranium Mining and Hydrometallurgy, University of South China, Hengyang 421001, China<&wdkj&>College of Public Health, Hengyang Medical School, University of South China, Hengyang 421001, Hunan, China
通讯机构：
[Zhongran Dai] K;Key Discipline Laboratory for National Defense for Biotechnology in Uranium Mining and Hydrometallurgy, University of South China, Hengyang 421001, China
摘要：
Photocatalysis holds promise for extracting uranium from aqueous solution. Nevertheless, conventional approaches generally rely on sacrificial agents and anaerobic conditions to maintain photocatalytic efficiency, which increases costs and causes secondary pollution. Herein, we introduce the design and synthesis of an S-scheme ZnIn2S4/g-C3N4 (ZISCN) heterojunction photocatalyst for the efficient removal of uranium via in-situ generating ZnIn2S4 on g-C3N4. Photoelectric characterization and theoretical calculation indicate that ZISCN boosts the absorption of visible light and promotes the effective separation and migration of charge carriers by forming an internal electric field (IEF) at the S-scheme heterojunction interface. This configuration integrates the strong reducing electrons of g-C3N4 and the potent oxidation holes of ZnIn2S4. Consequently, the as-synthesized ZISCN can efficiently remove uranium under an air atmosphere without the need for sacrificial agents and anaerobic conditions. The achieved U(VI) removal rate of 94.8 % surpasses that of ZnIn2S4 and g-C3N4 individually. Moreover, the photocatalytic extraction of U(VI) by ZISCN photocatalyst demonstrated excellent stability and anti-interference performance. After five cycles, the U(VI) removal rate remained above 85 %. Mechanism studies reveal that when electrons are generated by light in the ZISCN systems, they can reduce O2, leading to the formation of reactive species ·O2/H2O2. These species subsequently interact with U(VI), resulting in the precipitation of (UO2)O2·2H2O on the surface of ZISCN. This research provides valuable insights for the design of heterojunction photocatalysts for efficient, sacrificial agent-free uranium removal in ambient air environments.
摘要：
The concentration of metallic elements is closely associated with overall health. However, the discharge of untreated industrial wastewater can lead to metal -containing pollutants entering the human body through the food chain, disrupting the organism's homeostasis and posing a risk to human health. Covalent organic framework materials (COFs) have emerged as a novel porous material for detecting or adsorbing metal ions due to their unique pore structure, topological structure and flexible design. This paper summarizes the role, toxicity, and sources of metal ions related to human health, as well as the design, synthesis and performance of COFs fluorescent materials for detecting these elements. The interaction mechanism of different fluorescent COFs and metal ions are discussed. Additionally, the remaining challenges and prospects of COFs fluorescence sensors are provided. We believe this review will be useful in directing the development of fluorescent COFs towards metal ions. (c) 2024 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.
通讯机构：
[Li, L; Chen, SH; Zhen, DS ] U;Univ South China, Coll Publ Hlth, Hengyang Med Sch, Hunan Key Lab Typ Environm Pollut & Hlth Hazards, Hengyang 421001, Peoples R China.;Hunan Univ, State Key Lab Chemo Biosensing & Chem Engn, Changsha 410082, Peoples R China.
关键词：
Upconversion nanoparticles;Fluorescence resonance energy transfer;Uranyl;Deoxyribozyme;Hybrid chain reaction
摘要：
Anupconversion fluorescence sensing platform was developedwith upconversion nanoparticles (UCNPs) as energy donors and gold nanoparticles (AuNPs) as energy acceptors, based on the FRET principle. They were used for quantitativedetection ofuranyl ions (UO(2)(2+)) by amplifying the signal of the hybrid chain reaction (HCR). When UO(2)(2+) are introduced, the FRET between AuNPs and UCNPs can be modulated through a HCR in the presence of high concentrations of sodium chloride. This platform providesexceptional sensitivity, with a detection limit as low as 68pM for UO(2)(2+) recognition. We have successfully validated the reliability of this method by analyzing authentic water samples, achieving satisfactory recoveries (89.00%-112.50%) that are comparable to those of ICP-MS. These results indicate that the developed sensing platform has the capability to identify trace UO(2)(2+) in complex environmentalsamples.
摘要：
Deinococcus radiodurans (DR) exhibits strong resistance to ionizing radiation. In this study, by constructing a radiation-resistant genetically engineered strain overexpressing the Cs gene, the tolerance of the bacterium to aluminum ions was enhanced, thereby achieving the goal of microbial sustainable remediation of uranium-contaminated environments. Methods: 1. Extraction of the recombinant plasmid pRADK-Cs, transformation into DR, and verification. 2. Investigation of factors such as time and initial uranium concentration on the efficiency of uranium accumulation by the recombinant strain, characterized by changes in functional groups and surface morphology before and after accumulation using techniques such as scanning electron microscope. Conclusions: The recombinant strain Deino-Cs can reduce the inhibitory effect of aluminum ions on uranium accumulation capability, and it exhibits a higher uranium accumulation rate compared to the wild-type strain.
期刊：
International Journal of Biological Macromolecules,2024年259(Pt 1):129104 ISSN：0141-8130
通讯作者：
Liu, Y
作者机构：
[Liu, Yu; Zhang, Shaoqi; Li, Le; Zhen, Deshuai; Yang, Aofeng] Univ South China, Sch Publ Hlth, Hengyang Med Sch, Hunan Key Lab Typ Environm Pollut & Hlth Hazards, Hengyang 421001, Peoples R China.;[Liu, Yu; Zhang, Shaoqi; Zhen, Deshuai] Hunan Univ, Sch Chem & Chem Engn, State Key Lab Chemo Biosensing & Chemometr, Changsha 410082, Hunan, Peoples R China.;[Grimes, Craig A.] Flux Photon Corp, 5950 Shiloh Rd East, Alpharetta, GA 30005 USA.;[Liu, Yu] Univ South China, Sch Publ Hlth, Hengyang Med Sch, Hengyang 421001, Peoples R China.
通讯机构：
[Liu, Y ] H;Hunan Univ, Sch Chem & Chem Engn, State Key Lab Chemo Biosensing & Chemometr, Changsha 410082, Hunan, Peoples R China.;Univ South China, Sch Publ Hlth, Hengyang Med Sch, Hengyang 421001, Peoples R China.
关键词：
Covalent organic framework;Fluorescent probe;In vivo imaging
摘要：
Simple and accurate in vivo monitoring of Fe(3+) is essential for gaining a better understanding of its role in physiological and pathological processes. A novel fluorescent probe was synthesized via in situ solid-state polymerization of 3,4-ethylenedioxythiophene (PEDOT) in the pore channels of a covalent organic framework (COF). The PEDOT@COF fluorescent probe exhibited an absolute quantum yield (QY) 3 times higher than COF. In the presence of Fe(3+) the PEDOT@COF 475nm fluorescence emission, 365nm excitation, is quenched within 180s. Fluorescence quenching is linear with Fe(3+) in the concentration range of 0-960μM, with a detection limit of 0.82μM. The fluorescence quenching mechanism was attributed to inner filter effect (IEF), photoinduced electron transfer (PET) and static quenching (SQE) between PEDOT@COF and Fe(3+). A paper strip-based detector was designed to facilitate practical applicability, and the PEDOT@COF probe successfully applied to fluorescence imaging of Fe(3+) levels in vivo. This work details a tool of great promise for enabling detailed investigations into the role of Fe(3+) in physiological and pathological diseases.
通讯机构：
[Yang, SY; Li, L ] U;Univ South China, Sch Publ Hlth, Hengyang Med Sch, Dept Hlth Inspect & Quarantine, Hengyang 421001, Hunan, Peoples R China.;Univ South China, Hunan Key Lab Typ Environm Pollut & Hlth Hazards, Hengyang 421001, Peoples R China.
摘要：
Mercury is a highly toxic element that is widely present in all types of environmental media and can accumulate in living organisms. Prolonged exposure to high levels of mercury can lead to brain damage and death, so the detection of mercury is of great importance. In this study, a cost-effective and easy-to-operate electrochemical sensing method was successfully developed based on an amino-functionalized titanium-based MXene (NH(2)-Ti(3)C(2)T(x)) for the rapid and selective detection of Hg(2+) that could have a coordination effect with the -NH(2) group of NH(2)-Ti(3)C(2)T(x) to promote the efficient accumulation of Hg(2+). In this strategy, the NH(2)-Ti(3)C(2)T(x) was first modified on glassy carbon electrodes (GCE) to fabricate the electrochemical sensor. Benefiting from the excellent electrical conductivity, abundant active sites, and strong adsorption capacity performance of the NH(2)-Ti(3)C(2)T(x), the NH(2)-Ti(3)C(2)T(x) modified GCE (NH(2)-Ti(3)C(2)T(x)/GCE) exhibited satisfactory selectivity and enhanced square wave anodic stripping voltammetry (SWASV) measurement for the rapid detection of trace amounts of Hg(2+) in aqueous solutions. The electrochemical sensor was found to be capable of detecting Hg(2+) with a low detection limit of 8.27 nmol L(-1) and a linear range of 0.5 μmol L(-1) to 50 μmol L(-1). The response time of the electrochemical sensing method was 308 s. In addition, the electrochemical sensing method has good selectivity, repeatability and stability, and multiple heavy metal ions have no effect on its detection, with repeatability and stability RSDs of 1.68% and 1.43%, respectively. Furthermore, the analysis of practical water samples demonstrated that the developed method was highly practical for the actual determination of Hg(2+) with recoveries in the range of 99.22-101.90%.
作者机构：
[Tan, Yan; Liu, Jinquan; Shi, Jiao; Li, Le; Wang, Yating; Zhen, Deshuai; Liu, JQ; Zhou, Xiayu] Univ South China, Sch Publ Hlth, Hengyang Med Sch, Dept Hlth Inspect & Quarantine, Hengyang 421001, Hunan, Peoples R China.;[Tan, Yan; Liu, Jinquan; Shi, Jiao; Li, Le; Wang, Yating; Zhen, Deshuai; Liu, JQ; Zhou, Xiayu] Univ South China, Hunan Key Lab Typ Environm Pollut & Hlth Hazards, Hengyang 421001, Peoples R China.;[Tan, Yan; Liu, Jinquan; Shi, Jiao; Li, Le; Wang, Yating; Zhen, Deshuai; Liu, JQ; Zhou, Xiayu] Univ South China, Key Lab Hlth Hazard Factors Inspect & Quarantine, Hengyang 421001, Hunan, Peoples R China.;[Dai, Zhongran] Univ South China, Hunan Prov Key Lab Green Dev Technol Extremely Low, Hengyang 421001, Peoples R China.
通讯机构：
[Liu, JQ; Li, L ] U;Univ South China, Sch Publ Hlth, Hengyang Med Sch, Dept Hlth Inspect & Quarantine, Hengyang 421001, Hunan, Peoples R China.;Univ South China, Hunan Key Lab Typ Environm Pollut & Hlth Hazards, Hengyang 421001, Peoples R China.;Univ South China, Key Lab Hlth Hazard Factors Inspect & Quarantine, Hengyang 421001, Hunan, Peoples R China.
摘要：
In this study, we developed a simple and sensitive colorimetric sensing method for the detection of UO(2)(2+), which was built to release MB from the molybdenum disulfide with a phosphate group (MoS(2)-PO(4)) gated mesoporous silica nanoparticles functionalized phosphate group (MSN-PO(4)) with UO(2)(2+) chelating. In the presence of UO(2)(2+), MoS(2)-PO(4) can be effectively adsorbed onto the surface of MSN-PO(4) based on the coordination chemistry for strong affinity between the P-O bond and UO(2)(2+). The adsorbed MoS(2)-PO(4) was then utilized as an ideal gate material to control the release of signal molecules (MB) entrapped within the pores of MSN-PO(4), resulting in a detectable decrease in the absorption peak at 663 nm. This colorimetric sensing demonstrated the advantages of simplicity and easy manipulation and exhibited a linear response to the concentration of UO(2)(2+) within the range of 0.02-0.2 μM. The detection limit of UO(2)(2+) was determined to be 0.85 nM, which was lower than the limit (130 nmol L(-1)) set by the US Environmental Protection Agency. Furthermore, the proposed colorimetric sensing method has been utilized to determine UO(2)(2+) in samples of Xiangjiang River and tap water, and a high recovery rate was achieved. This method shows promising potential in preventing and controlling environmental pollution.
期刊：
Sensors and Actuators B-Chemical,2024年415:135875 ISSN：0925-4005
通讯作者：
Li, Le;Yang, Qinglai;Wu, GL
作者机构：
[Wang, Feirong; Liu, Yu; Li, Le; Yang, Qinglai; Wu, Gui-long; Wu, GL; Yang, QL; Yu, Wanying; Tan, Xiaofeng; Tan, Senyou] Univ South China, Dept Publ Hlth Lab Sci, Sch Publ Hlth, Affiliated Hosp 1,Hengyang Med Sch, Hengyang 421001, Hunan, Peoples R China.;[Wang, Feirong; Liu, Yu; Li, Le; Yang, Qinglai; Wu, Gui-long; Wu, GL; Yang, QL; Yu, Wanying; Tan, Xiaofeng; Tan, Senyou] Univ South China, Affiliated Hosp 1, Hengyang Med Sch, Dept Hepatopancreatobiliary Surg, Hengyang 421001, Hunan, Peoples R China.;[Yang, Qinglai; Wu, Gui-long; Tan, Xiaofeng] Univ South China, Canc Res Inst, Ctr Mol Imaging Probe, Hengyang Med Sch, Hengyang 421001, Hunan, Peoples R China.;[Yang, Qinglai; Wu, Gui-long; Tan, Xiaofeng] Hunan Prov Maternal & Child Hlth Care Hosp, Natl Hlth Commiss, Key Lab Birth Defect Res & Prevent, Changsha 410008, Peoples R China.;[Yang, Qinglai; Wu, Gui-long; Tan, Xiaofeng] Univ South China, Hengyang Med Sch, MOE Key Lab Rare Pediat Dis, Hengyang 421001, Hunan, Peoples R China.
通讯机构：
[Li, L; Wu, GL ; Yang, QL] U;Univ South China, Dept Publ Hlth Lab Sci, Sch Publ Hlth, Affiliated Hosp 1,Hengyang Med Sch, Hengyang 421001, Hunan, Peoples R China.;Univ South China, Affiliated Hosp 1, Hengyang Med Sch, Dept Hepatopancreatobiliary Surg, Hengyang 421001, Hunan, Peoples R China.
关键词：
NIR;Activated Probe;Cu(ii) ion quenching;H2S detection
摘要：
Human health, environmental contamination, and food safety are tightly associated with hydrogen sulfide (H2S). The safe and highly sensitive monitoring of H2S in tissues, organs, and blood has presented ongoing challenges. Herein, a novel near-infrared (NIR)-activated water-soluble molecular probe, denoted as IR820-TPY-Cu was developed for detecting hydrogen sulfide. This probe is built upon the fluorescent molecule IR820, a derivative of Indocyanine green (ICG). Upon reacting with H2S, IR820-TPY-Cu exhibits active fluorescence (670-750 nm), which is attributed to the Cu (II) ion quenching mechanism and substitution strategy. IR820-TPY-Cu exhibits selectively activated near-infrared fluorescence signal changes, a low detection limit of 0.114 mu M, and a rapid in vitro response (3 min) for H2S detection. Moreover, the biocompatible probe IR820-TPY-Cu not only quantitatively monitors H2S in environmental water and various food specimens (red wine, beer, meat, milk, and sweet potato) through colorimetric sensing but also successfully images endogenous and exogenous H2S in living cells, zebrafish, and mice. This research provides a promising approach for monitoring H2S in environmental contamination, ensuring food safety, and studying living systems.
作者机构：
[Yang, Shengyuan; Yang, SY; Liu, Yu; Liu, Chunlin; Li, Le; Zhen, Deshuai; Deng, Qiuhui] Univ South China, Sch Publ Hlth, Hengyang Med Sch, Hunan Key Lab Typ Environm Pollut & Hlth Hazards, Hengyang 421001, Peoples R China.;[Cai, Qingyun; Liu, Yu; Liu, Chunlin; Zhen, Deshuai; Deng, Qiuhui] Hunan Univ, Sch Chem & Chem Engn, State Key Lab Chemo Biosensing & Chemometr, Changsha 410082, Peoples R China.;[Grimes, Craig A.] Flux Photon Corp, Alpharetta, GA 30005 USA.
通讯机构：
[Yang, SY; Li, L; Liu, Y ] U;Univ South China, Sch Publ Hlth, Hengyang Med Sch, Hunan Key Lab Typ Environm Pollut & Hlth Hazards, Hengyang 421001, Peoples R China.;Hunan Univ, Sch Chem & Chem Engn, State Key Lab Chemo Biosensing & Chemometr, Changsha 410082, Peoples R China.
关键词：
amidoxime group;covalent organic frameworks;detection;knoevenagel;uranyl ion
摘要：
Monitoring and purification of uranium contamination are of great importance for the rational utilization of uranium resources and maintaining the environment. In this work, an olefin-linked covalent organic framework (GC-TFPB) and its amidoxime-modified product (GC-TFPB-AO) are synthesized with 3-cyano-4,6-dimethyl-2-hydroxypyridine (GC) and 1,3,5-tris(4-formylphenyl) benzene (TFPB) by Knoevenagel condensation. GC-TFPB-AO results in specificity for rapid fluorescent/smartphone uranyl ion (UO(2)(2+)) detection based on the synergistic effect of multifunctional groups (amidoxime, pyridine, and hydroxyl groups). GC-TFPB-AO features a rapid and highly sensitive detection and adsorption of UO(2)(2+) with a detection limit of 21.25 nM. In addition, it has a good recovery (100-111%) for fluorescence detection in real samples, demonstrating an excellent potential of predesigned olefin-linked fluorescent COFs in nuclear contaminated wastewater detection and removal.
作者机构：
[Tang, Xian; Han, Hai] Univ South China, Sch Nucl Sci & Technol, Hengyang 421001, Peoples R China.;[Li, Le] Univ South China, Sch Publ Hlth, Hengyang 421001, Peoples R China.;[Wang, Hongqing] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Wang, Hongqing] Univ South China, Hunan key Lab Design & Applicat Actinide Complexes, Hengyang 421001, Hunan, Peoples R China.
通讯机构：
[Tang, X ; Li, L ] U;Univ South China, Sch Nucl Sci & Technol, Hengyang 421001, Peoples R China.;Univ South China, Sch Publ Hlth, Hengyang 421001, Peoples R China.
摘要：
Utilizing elemental doping and defect engineering are effective means to enhance the efficiency of g-C3N4 materials for photocatalytic removal of uranium. In this investigation, we synthesized a defective g-C3N4 photocatalyst co-decorated with K+ doping and cyano groups (KHCN) through a straightforward one-step alkali etching process. The alkali etching not only enhances the specific surface area to improve the adsorption of uranium by KHCN but also significantly accelerates the photocatalytic removal of uranium through the introduction of K+ and cyano groups. The KHCN can almost completely remove 40 mg/L of U(VI) under air and visible LED light irradiation (pH 5.0, 298.15 K). Notably, the photocatalytic removal of U(VI) by KHCN demonstrated excellent selectivity and reusability. The mechanism studies reveal that alkali etching-induced introduction of K+ ions and cyano groups enhances visible light absorption, strengthens the efficiency of photogenerated carrier separation, and reduces the band gap. The activation of U(VI) in solution primarily occurs through photogenerated e- and center dot O2-, subsequently immobilizing as metastudtite ((UO2)O2 & sdot;2H2O). This study provides a viable approach for synthesizing highly efficient photocatalytic materials for uranium removal, leveraging synergistic doping and defect engineering.
摘要：
<jats:p>A novel near-infrared induced upconversion sensor for the detection of uranyl ions was successfully constructed using <jats:italic>β</jats:italic>-NaYF4: Yb, Tm, Gd upconversion nanoparticles (UCNPs) and specific DNAzyme. Characterization of the UCNPs@DNAzyme was conducted using XRD, TEM, FT-IR and
fluorescence testing, and it was shown that the <jats:italic>β</jats:italic>-NaYF4: Yb, Tm, Gd nanoparticles were successfully prepared (∼27 nm). Upon 980 nm excitation, the UCNPs@DNAzyme emitted green light at <jats:italic>λ</jats:italic>=475 nm. Furthermore, Förster resonance energy transfer was observed between
the UCNPs@DNAzyme (doner) and uranyl (acceptor) present on the substrate chain. This resulted in fluorescence quenching, which was used to quantify the concentration of uranyl. The developed method was found to be highly selective and sensitive, with a detection limit as low as 43 nM. This
method also demonstrated excellent specificity and sensitivity for the determination of uranyl in water samples, indicating its potential application in near-infrared fluorescence detection and imaging of uranyl <jats:italic>in vivo</jats:italic>.</jats:p>
