ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2020
·Vol. 412
·期 18
·4375-4382
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IF 3.637
Zhang Wen Jie,Liu Shi Gang,Zhang Xing Yue,Luo Hong Qun,Li Nian Bing
Ratiometric assays, which can effectively surmount external interference, have attracted extensive research interests. Herein, a novel ratiometric sensing platform for Hg 2+ is designed based on nitrogen-doped carbon dots (N-CDs) with two different optical signals. Under a single excitation, N-CDs have two emission peaks around 668 nm and 412 nm, which are second-order scattering and fluorescence, respectively. Upon the addition of Hg 2+ , the weak scattering emission at 668 nm can be increased apparently, while the strong fluorescence intensity at 412 nm is weakened. Moreover, the ratio of scattering intensity to fluorescence intensity is linearly dependent on Hg 2+ concentration (0.1–10 μM and 10–30 μM, respectively), and the detection limit is 66 nM. In addition, the ratiometric sensing mechanism is investigated in detail, which is due to the combined effect of aggregation-induced fluorescence quenching and scattering enhancement. Furthermore, the developed sensing approach holds a promising application for Hg 2+ detection in actual samples.
Graphical abstract
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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产品关联
DOI
PubMed
高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2022
·Vol. 414
·期 14
·4235-4244
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IF 4.478
Wang Jianping,Wang Wang,Yang Linlin,Zhao Jun,Han Guangmei,Yu Xiaoping,ShenTu Xuping,Ye Zihong
Chemical sensing for the sensitive and reliable detection of mercury(II) ions (Hg 2+ ) is of great importance in environmental protection, food safety, and biomedical applications. Due to the bio-enrichment property of Hg 2+ in organisms, it is particularly meaningful to develop an effective tool that can in situ and rapidly monitor the level of Hg 2+ in living organisms. In this work, we report ligand functionalized gold-silver bimetallic nanoclusters with bright red fluorescence as intracellular probes for imaging Hg 2+ in living cells and zebrafish. The bimetallic nanoclusters of DTT-GSH@Au/AgNCs (DG-Au/AgNCs) with strong fluorescence that benefited from the synergistic effect of Au and Ag atoms were obtained through a one-pot synthesis method, incorporating glutathione (GSH) and dithiothreitol (DTT) as the reducers and functionalized ligands. Attractively, the bright red fluorescence of DG-Au/AgNCs could be rapidly and selectively quenched by Hg 2+ within 1 min with a very low detection limit of 1.01 nM. Additionally, DG-Au/AgNCs had a great advantage in the detection of Hg 2+ in living cells and zebrafish owing to its notably strong red fluorescence at 665 nm, which could avoid effectively auto-fluorescence interference from the organism. Such easily prepared bimetallic fluorescent nanoclusters would be expected to provide a noninvasive and sensitive approach in the detection of heavy metals in situ for environmental protection. Graphical abstract
研究领域:
环境科学
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分析化学
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生物医学工程
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材料科学
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DOI
PubMed
高影响因子
MICROCHEMICAL JOURNAL
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2023
·
IF 4.8
Xue Li,Siying Xie,Cheng Qin,Sirui Liu,Fengli Su,Xing Zhang,Yue Chen,Bingzhi Li
Mercury ion (Hg 2+ ) is a highly toxic environmental pollutant, particularly harmful to human health, necessitating the development of analytical techniques with advanced performance to monitor its presence. Herein, we demonstrate the utility of fructose-stabilized DNA-copper nanoclusters (Fru@DNA-CuNCs) as a stable nanoprobe for the sensitive detection of Hg 2+ with a simplified procedure. Upon interaction with Hg 2+ , the fluorescence of Fru@DNA-CuNCs undergoes rapid quenching, which was caused by metallophilic interactions promoting electron transfer between Hg and Cu, changing the electron configuration of nanoclusters. This nanoprobe exhibits exceptional sensitivity, with a detection limit of 2.49 nM for Hg 2+ detection, and the detection process costs less than 20 min. Importantly, unlike other unstable CuNCs analogs, the incorporation of fructose enhances the stability of the Fru@DNA-CuNCs, which can maintain its performance for Hg 2+ detection after being stored for up to 4 weeks. This robustness makes it suitable for Hg 2+ monitoring without specialized and centralized facilities. To our knowledge, this is the first attempt to explore the analytical application of Fru@DNA-CuNCs, providing a facile, rapid, and stable synthetic biology-based sensing technique for Hg 2+ monitoring.
研究领域:
分析化学
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环境科学
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纳米技术
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DOI
高影响因子
BIOSENSORS & BIOELECTRONICS
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2021
·
IF 10.618
Mingliang Mei,Lixuan Mu,Sen Liang,Yuan Wang,Guangwei She,Wensheng Shi
The aptasensor , developed from the aptamer, has aroused wide concern in recent years owing to its high sensitivity and specificity. However, the quenching unit involved in the most of the aptasensors is indispensable to the fabrication of an aptasensor, which would undoubtedly increase the complexity of the device. In this study, a facile strategy was developed for construction of the quencher-free aptasensors, in which the quenching units can be omitted, and only an aptamer strand and a fluorophore are necessary. Distinguishable from the configuration of the traditional ones, the aptasensors developed in this work rationally employed the intrinsic quenching abilities of the analytes to directly regulate the fluorescence of the fluorophore. Furthermore, the aptamer strand as a discriminatory unit efficiently captured the corresponding analytes to around the fluorophores. As a result, the fluorescence of the aptasensor can be significantly sensitive to the analytes. The generality of the current design is evidenced by the successful fabrication of seven quencher-free aptasensors for Cu 2+ , Ag + , Hg 2+ , ATP and dopamine through 6-FAM labeling aptamers of Cu 2+ , Ag + , Hg 2+ , ATP, dopamine, 5-TAMRA and ROX labeling aptamers of Cu 2+ . Present strategy endows an aptasensor with a simple structure, high selectivity and fine sensitivity. The configuration of the quencher-free aptasensors fabricated in this work can be readily utilized for more aptasensors.
研究领域:
分析化学
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生物传感器
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分子生物学
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DOI
PubMed
高影响因子
MICROCHEMICAL JOURNAL
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2020
·
IF 3.594
Xiu-Fang Huang,Bing-Xue Ren,Chi-Fang Peng,Xin-Lin Wei,Zheng-Jun Xie
In this study, the fluorescence enhancement effect of guanine base on DNA-Cu/AgNCs was reported and fluorescent methods for the determination of Hg 2+ or Cu 2+ ion were established. The effect of adjacent and inserted guanine base (G) sequences in DNA template on the fluorescence intensity of DNA-Cu/AgNCs was investigated. It was found that G 5 sequence extended from the 5′ end of a typical C-riched DNA strand, 5′-CCCTTAATCCCC-3′ (DNA1), demonstrated fluorescence enhancement effect in the preparation of the DNA-Cu/AgNCs. Moreover, this G5-DNA-Cu/AgNCs can be used to determine Hg 2+ and Cu 2+ ions due to fluorescence quenching by the two metal ions while the DNA1-Cu/AgNCs only can determine Hg 2+ ions. Specific assays for Hg 2+ ions and Cu 2+ ions were established through masking Cu 2+ ions by EDTA and Hg 2+ ions by NaBH 4 , respectively. In Hg 2+ determination, a linear range from 5.0 nM to 40 nM was obtained with a detection limit of 1.0 nM. In Cu 2+ determination, a wide linear range from 0.01 µM to 5.0 µM was obtained with a detection limit of 5.0 nM. The recoveries of 89.6–106.8% for Cu 2+ ions and 90.6–106.2% for Hg 2+ ions were obtained in the measurements of Hg 2+ and Cu 2+ ions spiked lake samples, respectively. The results indicate the potential application of the DNA-Cu/AgNCs as a metal ions probes in real samples.
研究领域:
分析化学
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环境科学
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纳米技术
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生物化学
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产品关联
DOI
高影响因子
CARBOHYDRATE POLYMERS
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2022
·
IF 10.723
Ruyi Li,Fangyuan Liang,Xianyun Hu,Huiyang Bian,Chao Deng,Farzad Seidi,Baiyang Zhang,Huining Xiao,Yuqian Liu
In this work, a versatile cellulose nanocrystal‑carbon dots (CNC-CDs) architecture is prepared and applied in environmental remediation and biological sensing. The citric acid (CA) is employed to extract CNCs and in-situ synthesize blue-emissive CDs. The carboxyl-rich surface of CNC-CDs enables the chelation of Hg 2+ and fluorescence quenching of CDs, realizing the detection and adsorption of Hg 2+ with a film comprised of the architecture. The limit of detection (LOD) is measured as 12.8 nM with satisfying retention efficiency. The versatility of CNC-CDs is demonstrated by the fabrication of a fluorescence resonance energy transfer (FRET) sensor using m-tetrakis(4-sulfonatophenyl)porphine (TSPP) as FRET acceptor and Fe 3+ receptor. Fluorescence of the sensor is responsive to Fe 3+ in a ratiometric manner, which significantly contributes to the visualized and sensitive Fe 3+ detection (6.9 nM). In combination with excellent biocompatibility, the FRET sensor is capable of imaging intracellular Fe 3+ .
研究领域:
环境科学
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材料科学
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分析化学
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生物技术
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Houchao Shan,Shufeng Li,Zhen Yang,Xiaoxia Zhang,Yan Zhuang,Qian Zhu,Di Cai,Peiyong Qin,Jan Baeyens
Triazine-based N-rich covalent organic polymer (TBN-1) was prepared for effective removal and selective detection of Hg 2+ from model solutions. The π-π conjugated structure formed by alternating electron-deficient triazine group and electron-rich benzene group promotes the electron transfer and strong fluorescence. The ultra-high specific surface area and abundant metal complex groups provide excellent adsorption sites for heavy metals. The TBN-1 suspension has obvious fluorescence quenching effect when encountering Hg 2+ even when the solutions are treated with co-ions and humic acid. The merits of TBN-1 are unreservedly manifested when further testing the adsorption kinetics of TBN-1 for Hg 2+ removal. With the maximum adsorption capacity of 1630 mg g −1 , 99.99% of Hg 2+ can be removed within 20 min from a 10 ppm solution using TBN-1. The covalent organic polymer (COP) also exhibits a high stability in a wide range of pH and a significant selectivity for Hg 2+ . About 99.9% Hg 2+ can be adsorbed in acidic, co-ions competitive and humic acid contaminated solutions. The TBN-1 can be also reused for at least 5 cycles with acceptable Hg 2+ adsorption capacity retention. The mechanism for the excellent Hg 2+ adsorption performance of TBN-1 is revealed by coupling physico-chemical model fitting, chemical computation, and experimental characterization, which indicates the coordination and cation-π effects and high electron density of the material to facilitate its complexation with Hg 2+ . This work offers new prospects for the application of triazine-based COPs for environmental remediation.
研究领域:
环境科学
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材料科学
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分析化学
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水处理
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF ANALYTICAL CHEMISTRY
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2022
·
IF 1.193
Ri WANG,Chen-Yu XIONG,Yong XIE,Ming-Jie HAN,Yu-Hao XU,Chao BIAN,Shan-Hong XIA
Mercury ions (Hg 2+ ) are highly toxic and can cause serious harm to the environment and human health. In this study, we prepared a novel electrochemical sensor based on an electrode coated with chitosan/graphene oxide/molybdenum disulfide/Au nanoparticles (chitosan/GO/MoS 2 /AuNPs) and thymine-Hg 2+ -thymine base pair to detect trace Hg 2+ in water. This method effectively utilized the affinity of MoS 2 to immobilize deoxyribonucleic acid (DNA) on the electrode surface and enabled the amplification of the electrochemical signals detected by the sensor. The specific binding of the thymine-Hg 2+ -thymine base pair and the electrochemical activity of MoS 2 successfully reduced the detection limit of Hg 2+ and rendered it interference resistant. In the presence of Hg 2+ , a double-stranded structure was formed on the electrode after the interaction between Hg 2+ and DNA, which caused the change of the oxidation current signal of the electrode surface. The sensor showed good linearity ranging from 0.01 μg/L to 4 μg/L with a correlation coefficient of 0.991, and the limit of detection was found to be 5.8 ng/L. This portable chitosan/GO/MoS 2 /AuNPs modified electrode showed satisfactory recovery in tap water samples, thus demonstrating its potential for application in trace Hg 2+ detection.
研究领域:
环境科学
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分析化学
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材料科学
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电化学
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产品关联
DOI
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2021
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IF 4.098
Yanyun Zou,Qingli Chai,Ting Zhu,Xiaoxiao Yu,Guobin Mao,Ningxing Li,Jinyang Chen,Guosong Lai
In this work, an environmentally-friendly and cost-effective enzyme mimic was obtained by facile one-pot preparation of chitosan/Cu/Fe (CS/Cu/Fe) composite. This composite exhibited significantly enhanced oxidase-mimicking activity during catalyzing the oxidation of 3, 3′, 5, 5′-tetramethylbenzidine (TMB). The CS/Cu/Fe composite was comprehensively characterized and the possible catalytic mechanism was reasonably explored and discussed. Benefiting from the thermal stability and the compatibility with carbohydrate, the CS/Cu/Fe composite was further integrated with agarose hydrogel to fabricate a portable analytical tube containing oxidase mimic. Based on the inhibition of the catalytic oxidation of TMB in the presence of cysteine, as well as the recovery of oxidase-like activity of CS/Cu/Fe due to the specific complexation of cysteine and mercury ion (Hg 2+ ), the rapid colorimetric detection of Hg 2+ was successfully carried out in the analytical tube. This colorimetric method showed good linear response to Hg 2+ over the range from 40 nM to 8.0 μM with a detection limit of 8.9 nM. The method also revealed high selectivity and satisfactory results in recovery experiments of Hg 2+ detection in tap water and lake water. Furthermore, it was found that the effective removal of Hg 2+ could be realized in the analytical tube based on efficient Hg 2+ adsorption by CS/Cu/Fe composite and agarose hydrogel. This study not only prepared a robust and low-cost enzyme mimic, but also proposed a smart strategy to simultaneously monitor and remove toxic Hg 2+ from contaminated water.
研究领域:
环境科学
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分析化学
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材料科学
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水处理
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DOI
PubMed
高影响因子
TALANTA
·
2018
·
IF 4.244
Fen Ma,Yu Chen,Yinchang Zhu,Jiawei Liu
A new electrogenerated chemiluminescence (ECL) biosensor is fabricated for the determination of mental ion incorporating DNA three-way junction structure (DNA-TWJ). As a model system, Hg 2+ was chosen as an analyte. The ECL biosensor was fabricated by covalently coupling Hg 2+ special DNA-TWJ tagged with ruthenium (II) complex (Ru) (named TW/Ru-J1) to the surface of glassy carbon electrode that had been covalently modified with 4-aminobenzoic acid via electrochemical oxidations . Upon binding of Hg 2+ to the TW/Ru-J1, the confirmation of TW/Ru-J1 changed and induced Ru away from surface of electrode and thus led to a low ECL signal. The signal linearly decreases with the concentration of Hg 2+ in the range from 0.1 pM to 10 pM with a detection limit of 0.04 pM This study could be easily extended to various analytical platforms for the detection of many kinds of analytes or their interactions such as DNA/RNA, DNAzyme/target, aptamer/target, and antibody/antigen.
研究领域:
分析化学
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环境科学
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生物化学
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纳米技术
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产品关联
DOI
PubMed
高影响因子
TALANTA
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2018
·
IF 4.244
Qiang Zou,Xin Li,Tao Xue,Jia Zheng,Qi Su
A conceptually new class of DNA logic gates for Hg 2+ and Pb 2+ ion simultaneous detection has been constructed based on the activity of DNAzyme dependent on metal ions . For sensitive and specific detection of Hg 2+ and Pb 2+ ions, we demonstrate a surface-enhanced Raman scattering (SERS)-active platform by employing the oligonucleotide-functionalized and gold coated polystyrene microspheres (PSMPs). In this work, Hg 2+ and Pb 2+ were used as the input, and the SERS signals were the output. Hg 2+ ions were captured by a mismatched T-Hg-T bridge. Pb 2+ ions were bound to 8–17DNAzyme to break the cleavage substrate. The limit of detection (LOD) of Hg 2+ is 0.1 nmol L −1 and Pb 2+ is 1.0 nmol L −1 , which is far below the limit of 10.0 ppb (31 nmol L −1 ) and 10.0 ppm (3.02 × 10 4 nmol L −1 ) for drinking water stipulated by the World Health Organization. Additionally, this system has the potential to be ideal candidates for intelligent DNA calculator design applications. Furthermore, the designed strategy could be extended to other multiplex metal ions that can be combined with DNA molecules, and can be applied to many other fields such as environmental detection, toxin detection and liquid analysis.
研究领域:
分析化学
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环境科学
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生物化学
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纳米技术
✓ 已验证
DOI
PubMed
高影响因子
WATER RESEARCH
·
2024
·
IF 11.4
Yurong Wu,Guangliang Liu,Xiaoquan Liu,Yuxiang Mao,Yingying Guo,Yanwei Liu,Liuchao Zhu,Yongguang Yin,Yong Cai,Guibin Jiang
Ethylmercury (EtHg), similar to methylmercury (MeHg), is highly neurotoxic and bioaccumulative. Although recent studies suggested its occurrence in natural soils and sediments, the common propylation derivatization for EtHg analysis might generate EtHg artifacts, potentially leading to its overestimation in environmental samples. Furthermore, the extensive environmental prevalence of EtHg remains unverified, keeping its importance largely uncertain. This study investigated the formation of EtHg artifacts during propylation derivatization, evaluating artifacts formation and recoveries under different extraction methods with real samples, and confirmed the widespread occurrence of EtHg in Chinese wetlands. EtHg artifacts were obviously present during the propylation derivatization and strongly dependent on the levels of Hg 2+ (0.1–10 ng) in the derivatization solution (R² = 0.99), accounting for 1.38–2.14% of Hg 2+ . CuSO 4 -HNO 3 CH 2 Cl 2 extraction (effectively removing Hg 2+ ) combined with propylation derivatization offers excellent recovery (81–86%) and low artifacts (< LOD: 1.98 × 10 −4 ng/g) for EtHg measurement in soils/sediments, with results aligning with those from online solid phase extraction-high performance liquid chromatography-inductively coupled plasma mass spectrometry (R 2 = 0.99). Additionally, we observed the occurrence of EtHg in soil and sediment samples across 14 Chinese wetlands, with concentrations varying from 6.08 to 171 pg/g, similar to MeHg concentrations at some sites. EtHg positively correlates with MeHg, total Hg, and total organic carbon across all samples, indicating a possible biological formation. These findings help better understand and predict the prevalence of EtHg in wetlands and its key role in environmental Hg cycle.
研究领域:
环境科学
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分析化学
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生态毒理学
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）