ANALYTICA CHIMICA ACTA
·
2024
·
IF 5.7
Xiaolai Zhang,Fangli Li,Jingbo Chao,Zhicai Li,Guimin Zhang,Lihai Zhai,Ligang Hu,Heping Jiao,Zhenhua Wang
Background Trace levels of organic and inorganic lead and mercury species in the environment, including divalent lead (Pb 2+ ), trimethyllead (TML), divalent mercury (Hg 2+ ), monomethylmercury (MeHg), and ethylmercury (EtHg), are highly toxic to humans and ecology. It is of great importance for speciation of lead and mercury to evaluate the toxicity of lead and mercury and their biogeochemistry in the environment. However, simultaneous multi-elemental enrichment and speciation at trace level remains a challenge. There are few reports of simultaneous magnetic solid-phase extraction (MSPE) of organic and inorganic lead and mercury species at trace level in the real water. Results In this work, a novel core-shell magnetic hydrazine-linked covalent organic frameworks (Fe 3 O 4 @COF-TCH) was prepared for the first time by grafting hydrazine-linked COFs on the Fe 3 O 4 nanoparticles. Fe 3 O 4 @COF-TCH with abundant thione and imino groups has strong adsorption for lead and mercury species. Based on it, a simple and practical magnetic solid-phase extraction high-performance liquid chromatography-inductively coupled plasma mass spectrometry (MSPE-HPLC-ICP-MS) method was developed for extraction and determination of trace lead and mercury species, including Hg 2+ , MeHg, EtHg, Pb 2+ and TML. The limits of detection (3δ) of the developed method were 0.08, 0.81, 0.90, 0.56 and 0.88 ng L −1 with the enrichment factors (EFs) of 384, 376, 379, 389 and 360-fold for Pb 2+ , TML, Hg 2+ , MeHg and EtHg, respectively. The high accuracy and reproducibility have been proved by the spiked recoveries (94.4–103 %) in real samples. Significance The proposed method with simple operation and high sensitivity has been successfully applied to simultaneous speciation of lead and mercury at trace levels in the water samples with complicated matrices, including underground water, surface water, sea water. Meanwhile, it has the advantages of cost-saving, labor-saving and time-saving and is suitable for the investigation and risk assessment in water. The development of MSPE-HPLC-ICP-MS method provides ideas and guidance for the simultaneous multi-elemental enrichment and speciation.
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
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2024
·
IF 6.7
Wenxiao Tang,Beibei Chen,Man He,Gaofei Song,Yonghong Bi,Bin Hu
Understanding the interactions between mercury and microalgae, especially the interactions between inorganic mercury (IHg) and extracellular polymeric substances (EPS, a protective barrier between cells and their external environment), is essential for elucidating mercury’s toxicological mechanisms. Given the inherent cell heterogeneity, a novel analysis system of an online viscoelastic fluid focusing chip-time-resolved analysis inductively coupled plasma mass spectrometry has been developed to investigate the bioaccumulation of HgS nanoparticles and Hg2+ in single Microcystis aeruginosa (M. aeruginosa) cells, exploring the interaction mechanisms between HgS/Hg2+ accumulation in algal cells and EPS. The single-cell analysis results reveal minimal bioavailability of HgS within algal cells, with mercury’s toxicity to M. aeruginosa being species-dependent. Notably, algal cells exhibited more heterogeneity in HgS uptake than in Hg2+ uptake. Under Hg2+/HgS stress, M. aeruginosa cells with EPS removed (EPS-R algal cells) showed an increased level of bioaccumulation of mercury compared to those with EPS (EPS-C algal cells), highlighting the critical role of EPS in mercury bioaccumulation. Overall, the designed viscoelastic fluid microfluidic focusing chip integrates focusing and cleaning functions, featuring easy fabrication, simple operation, low sample loss, and relatively high throughput. Under the optimal conditions, the sample throughput is 1195 min–1 and the cell recovery is 90%. Besides, this research offers novel insights into the interaction mechanisms between Hg2+/HgS and EPS in microalgal cells and unveils the specific toxic effects of Hg2+/HgS on M. aeruginosa at the single-cell level, contributing to a deeper understanding of mercury’s ecological and toxicological impact in aquatic environments.
研究领域:
环境科学
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毒理学
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分析化学
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DOI
PubMed
高影响因子
ANALYTICA CHIMICA ACTA
·
2019
·
IF 5.256
Shiwei Yang,Danyu Zhang,Heyong Cheng,Yuanchao Wang,Jinhua Liu
For the past several decades, lots of adsorbent nanomaterials have been adopted for the enrichment of mercuric compounds. In this paper, graphene oxide bounded silica particles were employed as the absorbent for online preconcentration of Hg(II), methylmercury (MeHg) and ethylmercury (EtHg) by solid phase extraction . The adsorbent offered satisfactory adsorption capacities of 40.7 for Hg(II), 91.4 for MeHg and 103.8 mg g −1 for EtHg. Enrichment conditions such as type, concentration and volume of conditioning and eluting reagents were optimized. The pH, volume and flow rate of sample were also optimized. High enrichment factors (1963, 1881 and 1794 for Hg(II), MeHg and EtHg, respectively) were obtained with 10 mL sample (adjusted to pH 4–7) at 10 mL min −1 flow rate, 5 μL of 10 mM benzoic acid for elution and 4 mL of 1 mM 4-phenyl-3-aminothiourea for preconditioning. The detection limits obtained were downscaled to be 0.005 for Hg(II), 0.006 for MeHg and 0.009 ng L −1 for EtHg with relative standard deviations of all the analytes below 5%. Standard reference material and spiked water samples were analyzed for validating the method with satisfactory recoveries of 89–106%. The present method was successfully applied to determine mercury compounds in drinking water , and river and tap water , in which Hg(II), MeHg and EtHg were presented below the China's drinking standard limit of 1 μg L −1 .
研究领域:
环境科学
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分析化学
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DOI
PubMed
高影响因子
TALANTA
·
2021
·
IF 6.057
Wen-Jing Wei,Yuan Yang,Xin-Yuan Li,Peng Huang,Qiang Wang,Ping-Jian Yang
Silver Nanoparticles (Ag-NPs), an emerging type of pollutant, might occur various physical and chemical transformations, which would affect its environmental fate, transformation and biological effects. Sulfurization is the most common conversion of Ag-NPs, accompanied by the formation of nano-silver sulfide (Ag 2 S-NPs). The method of Ag 2 S-NPs analysis and characterization is of great significance for assessing the environmental risks of Ag. In this study, cloud point extraction (CPE) and Single Particle-Inductively Coupled Plasma-Mass Spectrometry (SP-ICP-MS) were used in combination to establish a simple and reliable analysis method to quantify Ag 2 S-NPs in water, with the morphology unchanged. Non-Ag 2 S-NPs were dissociated into Ag + firstly, and Ag 2 S-NPs and Ag + were separated by CPE, followed by SP-ICP-MS analysis. The extraction rate based on particle number concentration was between (76.19 ± 0.56) % to (106.35 ± 0.00) % in environmental waters. Compared with the (76.96 ± 2.18) nm Ag 2 S-NPs spiked, the particle size extracted increased slightly with (94.19 ± 2.72) nm- (97.25 ± 0.22) nm as the large-size Ag 2 S-NPs originally presented in waters, instead of agglomeration. This method could be generally applicable to the analysis of Ag 2 S-NPs in waters, and provide ideas for other metal sulfide nanoparticles (MS-NPs), which has certain significance.
研究领域:
环境科学
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分析化学
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产品关联
DOI
PubMed
高影响因子
TALANTA
·
2019
·
IF 4.916
Guangyang Xiao,Beibei Chen,Man He,Xiaoting Li,Bin Hu
In this work, a simple, sensitive and specific assay for DNA was proposed by combining inductively coupled plasma mass spectrometry (ICP-MS) detection with gold nanoparticle (AuNPs) amplification and isothermal circular strand-displacement polymerization reaction (ICSDPR). First, AuNPs were decorated with hairpin-structured DNA (HP-DNA) through Au–S bond to form the AuNPs probe. The ICSDPR was conducted on AuNPs probe in a homogeneous phase to realize the dual amplification and simplify the analytical process at the same time. By using a biotin modified primer, AuNPs were connected with biotins after the ICSDPR, then captured by the streptavidin modified magnetic beads (SA-MBs), and finally detected by ICP-MS. Many key factors including probe volume, hybridization time, polymerase amount, primer concentration, enzyme reaction time, SA-MBs capture time and desorption time were optimized. Under the optimized condition, the proposed method could detect target DNA as low as 45 zmol (8.9 fM in 5 μL) in a relative short time (about 4.5 h) with good specificity, and the linear range of this method is 0.1–10000 pM, the relative standard deviations are in the range of 3.6–6.4%. The proposed method was applied for determination of target DNA in human serum samples, the recovery for the spiked human serum samples is in the range of 84–120%. It demonstrates a good application potential of the developed method for biological studies and clinical diagnosis of human pathogenic diseases.
研究领域:
分析化学
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纳米技术
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生物医学工程
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分子生物学
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临床诊断
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DOI
PubMed
高影响因子
MICROCHEMICAL JOURNAL
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2026
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IF 5.2
Beili Wang,Wei Gao,Liang Yang
An Exo-III-triggered target-reconstructed DNAzyme walker enables ultrasensitive multiplex miRNA detection. • Cascade amplification integrates Exo-III recycling, polymerase/endonuclease cycling, and DNAzyme walking. • Orthogonal Pt, Ir, Rh tags allow simultaneous ICP-MS quantification of three miRNAs without spectral cross-talk. • Detection limits reach 0.15 fM (miR-21), 0.32 fM (miR-1246), and 0.26 fM (miR-20a) with excellent linearity. • The method discriminates single-base mismatches and performs well in diluted human serum (92–108% recovery). Cervical cancer remains a leading cause of cancer-related mortality among women, and the prognosis of patients after radiotherapy varies considerably due to differences in tumor radiosensitivity and treatment response. Reliable biomarkers for post-radiotherapy prognosis are therefore critically needed. MicroRNAs (miRNAs) have emerged as promising non-invasive indicators, yet accurate detection is hindered by their low abundance and the lack of multiplexing capability in conventional methods. Herein, we report a highly sensitive and specific platform for simultaneous detection of three cervical cancer radiotherapy-associated miRNAs (miR-21, miR-1246, and miR-20a) by integrating an Exo-III-triggered target-reconstructed DNAzyme walker with inductively coupled plasma mass spectrometry (ICP-MS). The strategy employs a structurally locked DNA walker that is sequentially activated through Exo-III-mediated target recycling and DNA polymerase/endonuclease-assisted cyclic amplification, ultimately unleashing a DNAzyme walker to cleave element-labeled substrates. Using orthogonal platinum group element tags (Pt, Ir, Rh), the released tags are quantified by ICP-MS without spectral cross-talk. The method achieves detection limits as low as 0.15 fM, 0.32 fM, and 0.26 fM for miR-21, miR-1246, and miR-20a, respectively, with excellent single-nucleotide discrimination and negligible cross-reactivity. Successful spike-recovery experiments in diluted human serum validate its practical feasibility. This cascade amplification strategy offers a robust, multiplex, and ultrasensitive tool for non-invasive liquid biopsy-based prognostic assessment of post-radiotherapy cervical cancer, and can be readily adapted for other disease-related miRNA panels. Download: Download high-res image (121KB) Download: Download full-size image
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DOI
高影响因子
Nanoscience and Nanotechnology Letters
·
2019
·Vol. 11
·期 5
·638-644
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IF 0
Jiang Pengfei,Haji Chomba,Ye Xiufang,Chang Menglei,Li Wenjun,He Xuliang,Chen Dongchu,Nie Libo
An inductive coupled plasma mass spectrometry (ICP-MS) method based on gold nanoparticles (AuNPs) and bio-barcode signal amplification was presented for the sensitive detection of gastric cancer related gene. The target DNA, magnetic nanoprobes and SiO2/AuNPs barcode probes
were hybridized to form a "sandwich" structure, then a large amount of AuNPs which were amplified by bio-barcode technology were detected by ICP-MS. This method presented a limit of detection as low as 1 fM. The ratio of the background-subtracted 197 Au signals for totally complementary
DNA, single-base mismatched DNA, double-base mismatched DNA and totally mismatched DNA was 115:30:16:1, respectively. It's suggested that the complementary and mismatched DNA can be distinguished clearly. This novel ICP-MS biosensor is prospective in DNA detection with high sensitivity and
specificity.
研究领域:
分析化学
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分子生物学
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癌症研究
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纳米技术
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DOI
MOLECULES
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2022
·Vol. 27
·期 22
·7683
·
IF 4.927
Meng-Fei Guo,Huan-Huan Zhang,Ping Zhong,Jin-Di Xu,Shan-Shan Zhou,Fang Long,Ming Kong,Qian Mao,Song-Lin Li
Cicadae Periostracum (CP) is a traditional Chinese medicinal herb derived from the slough that is molted from the nymph of the insectCryptotympana pustulataFabricius. Washing with water to remove residual silt is a primary processing method of CP that is recommended by the Chinese Pharmacopoeia, but how washing methods affect the quality and bioactivity of CP is unknown. In this study, the quality and bioactivity of non-washed CP (CP-NW), post-molting-washed CP (CP-WAT), and pre-molting-washed CP (CP-WBT) were comparatively investigated. The quality of these CP samples was evaluated in terms of the UPLC-QTOF-MS/MS-based chemical profiling and semi-quantification of 39N-acetyldopamine oligomers (belonging to six chemical types), the HPLC-UV-based quantification of 17 amino acids, the ICP-MS-based quantification of four heavy metals, and the contents of ash; the bioactivities of the samples were compared regarding their anti-oxidant and anti-inflammatory activities. It was found that, compared with CP-NW, both CP-WBT and CP-WAT had significantly lower contents of ash and heavy metals. Moreover, compared with CP-WAT, CP-WBT contained lower levels of total ash, acid-insoluble ash, and heavy metals and higher contents ofN-acetyldopamine oligomers and amino acids. It also had enhanced anti-oxidant and anti-inflammatory activities. A Spearman’s correlation analysis found that the contents ofN-acetyldopamine oligomers and free amino acids were positively correlated with the anti-oxidant/-inflammatory activities of CP. All these results suggest that pre-molting washing can not only remove the residual silt but can also avoid the loss of the bioactive components and assure higher bioactivities. It is concluded that pre-molting washing could enhance the quality and bioactivity of CP and should be a superior alternative method for the primary processing of qualified CP.Keywords:Cicadae Periostracum;primary processing;pre/post-molting washing;quality;bioactivity
研究领域:
药用植物学
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药物化学
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中药学
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分析化学
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DOI
PubMed
高影响因子
JOURNAL OF ANALYTICAL ATOMIC SPECTROMETRY
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2011
·Vol. 26
·期 6
·1191-1197
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IF 4.372
Jing-Min Liu,Xiu-Ping Yan
An ultrasensitive method for simultaneous determination of cytochrome c (cyt-c) and insulin was developed by combining aptamer-based bioassay and immunoassay, multielement-tagging and inductively coupled plasma mass spectrometry (ICP-MS). Aptamer-modified gold nanoparticles (apt-AuNPs) and antibody-modified silver nanoparticles (ab-AgNPs) were employed as specific element tags for cyt-c and insulin, respectively. The prepared surface-functionalized magnetic microparticles (MMPs) were used for efficient and fast magnetic separation. The bioassay conditions were carefully optimized, including the amount of MMPs, the concentration of AuNPs and AgNPs, and the reaction time. Under optimal conditions, the developed method gave a linear range of 0.1–20 nM for cyt-c and 0.2–40 nM for insulin, a detection limit (3s) of 1.5 fmol (30 pM in 50 μL) for cyt-c and 5.5 fmol (110 pM in 50 μL) for insulin. The precision (relative standard deviation) for six replicate determinations of cyt-c (0.6 nM) and insulin (2.0 nM) was 6.6%, and 6.0%, respectively. The present method exhibits good specificity with recoveries from 87% to 98% for spiked cyt-c and insulin in human serum samples. The methodology demonstrated here provides a new possibility for bioassays and clinical diagnoses, which has potential for simultaneous determination of two or more low-abundance biomarkers of interest via multi-element tags.
研究领域:
生物分析化学
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分子诊断
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纳米生物技术
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临床检验医学
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蛋白质组学
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DOI
高影响因子
ANALYTICAL LETTERS
·
2021
·
IF 2.329
Zhaoxue Zhang,Yi Lu,Haipu Li,Nan Zhang,Junfei Cao,Bo Qiu,Zhaoguang Yang
The simultaneous separation and determination of inorganic trivalent antimony Sb(III) and pentavalent antimony Sb(V) in plant, soil, and sediment samples was carried out by high performance liquid chromatography – inductively coupled plasma – mass spectrometry (HPLC-ICP-MS). The chromatographic conditions (composition and concentration of competing ion, pH value and flow rate of mobile phase) and the operating parameters for inductively coupled plasma – mass spectrometry were optimized by single factor experiments. The separation of the Sb species was achieved within 6 min using the optimized chromatographic conditions. The detection limits of the method were 0.016 μg/L and 0.021 μg/L for Sb(III) and Sb(V), respectively. The retention times of Sb(V) and Sb(III) were 2.7 min and 4.5 min, respectively. The relative standard deviations for replicate measurements (n = 6) of low (5 μg/L), medium (20 μg/L), and high (40 μg/L) concentrations of Sb(III) and Sb(V) were less than 4%. The results of spiking and recovery experiments for the extracting solutions of soil, sediments, and plants showed that the spiked recoveries of the two species ranged from 92% to 103%. This method has been used to determine the antimony species in extracts of environmental samples.
研究领域:
环境科学
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分析化学
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产品关联
DOI
高影响因子
TALANTA
·
2024
·
IF 5.6
Yongsheng Zhang,Jian Yuan,Rui Gao,Yang Zhao,Zefu Ye,Zhujun Zhu,Peihua Zhang,Lei Zhang,Wangbao Yin,Suotang Jia
Ash content, as a crucial indicator of coal quality, its rapid and accurate determination is pivotal to improve the energy utilization of coal and reduce environmental pollution. Traditional spectroscopic methods face significant challenges in acquiring accurate information from coal samples due to the notorious matrix effects arising from their complex composition, vast molecular structure, and diverse coal types. In this study, the feasibility of total reflection X-ray fluorescence (TXRF) combined with partial least squares (PLS) for the determination of coal ash was firstly investigated based on the TXRF being unaffected by matrix effects. Firstly, coal samples were prepared as suspensions, and the effects of sample particle size and different dispersants on the results of TXRF analyses were evaluated. The accuracy and applicability of the chosen sample preparation strategies were further validated using inductively coupled plasma mass spectrometry (ICP-MS) and two certified reference materials (CRMs). Subsequently, based on the analysis of 19 coal samples, the impact of three different predictive variables on the performance of the PLS model was investigated: (a) TXRF full spectrum normalized by the net intensity of the internal standard; (b) net intensity of characteristic peaks for 12 elements (Al, Si, K, Ca, Ti, Fe, Cr, Mn, Cu, Ni, and Sr) normalized by the net intensity of the internal standard; (c) concentrations of the aforementioned 12 elements. The results demonstrate that the PLS model constructed usingthe TXRF full spectrum normalized by the net intensity of the internal standard exhibits the best predictive capabilities, with the determination coefficient of calibration set (R 2 ) and mean square error (MSE) of the prediction set reaching 0.9736 and 0.99 %, respectively. Moreover, the measurement accuracy of this model was six times greater than that obtained with traditional X-ray fluorescence (XRF). Presented analytical results display the possibilities of combining TXRF with PLS for coal quality evaluation.
研究领域:
分析化学
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环境科学
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能源资源
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产品关联
DOI
PubMed
高影响因子
Journal of Food Measurement and Characterization
·
2021
·Vol. 15
·期 6
·4849-4857
·
IF 2.431
Xu Yi,Kutsanedzie Felix Y. H.,Ali Shujat,Wang Pingyue,Li Chunyan,Ouyang Qin,Li Huanhuan,Chen Quansheng
Lead ion (Pb 2+ ) accumulation in food consumed by humans and animals possess health threats and effects. The development of a senor for its monitoring at its minutest accumulation in edible materials becomes an antidote to safeguarding human lives. A fabricated fluorescence-based sensor made of carboxyl modified upconversion nanoparticles (UCNPs), gold nanorods (GNRs), and cysteamine (Cys) were used as energy donor, receptor and a bridge respectively for the rapid sensing of Pb 2+ in Matcha. The UCNPs-Cys-GNRs sensor showed weak fluorescence signals due to the FRET, and was inhibited in the presence of Pb 2+ to form a complex with Cys, and the consequent recovery of fluorescence signals. Under optimized conditions, a good linear relationship was established between the relative fluorescence intensity and Pb 2+ concentrations from 1 to 100 μM with a low detection limit (LOD) of 0.5 μM. The developed sensor was applied to detect Pb 2+ in Matcha samples with recoveries within 93.99—102.16% and relative standard deviations (RSD) < 8%. Satisfactory results (p > 0.05) were obtained upon validation using a standard inductively coupled plasma mass spectrometry (ICP-MS).
研究领域:
分析化学
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环境科学
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食品科学
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纳米技术
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）