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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2022 · IF 11.357

Extraction and Quantification of Nanoparticulate Mercury in Natural Soils

Weiping Cai,Yujun Wang,Yu Feng,Peng Liu,Shuofei Dong,Bo Meng,Hua Gong,Fei Dang

Nanoparticulate mercury (Hg-NPs) are ubiquitous in nature. However, the lack of data on their concentration in soils impedes reliable risk assessments. This is due to the analytical difficulties resulting from low ambient Hg concentrations and background interferences of heterogeneous soil components. Here, coupled to single particle inductively coupled plasma-mass spectrometry (spICP-MS), a standardized protocol was developed for extraction and quantification of Hg-NPs in natural soils with a wide range of properties. High particle number-, particle mass-, and total mass-based recoveries were obtained for spiked HgS-NPs (74–120%). Indigenous Hg-NPs across soils were within 107–1011 NPs g–1, corresponding to 3–40% of total Hg on a mass basis. Metacinnabar was the primary Hg species in extracted samples from the Wanshan mercury mining site, as characterized by X-ray absorption spectroscopy and transmission electron microscopy. In agreement with the spICP-MS analysis, electron microscopy revealed comparable size distribution for nanoparticles larger than 27 nm. These indigenous Hg-NPs contributed to 5–65% of the measured methylmercury in soils. This work paves the way for experimental determinations of indigenous Hg-NPs in natural soils, which is critical to understand the biogeochemical cycling of mercury and thereby the methylation processes governing the public exposure to methylmercury.

研究领域: 环境科学 · 分析化学
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JOURNAL OF CHROMATOGRAPHY A · 2022 · IF 4.601

Simultaneous solvent extraction and quantification of eleven amine compounds related to Chemical Weapon Convention in soils via hydrophilic interaction liquid chromatography-tandem mass spectrometry

Pei-Yu Jiang,Ling Yuan,Shi-Lei Liu,Qiao Lv,Hui-Lan Yu,Long-Hui Liang,Yang Yang,Chang-Cai Liu

The detection of Chemical Weapon Convention (CWC)-related amine compounds including the precursors or degradation products of V-type organophosphorus nerve agent, nitrogen mustard and 3-quinuclidinyl benzilate is an important aspect for verifying their intact chemical warfare agents. This work focuses on the development of a novel formulation for the simultaneous solvent extraction of eleven CWC-related amine compounds, from the four-type soil matrices including environmental standard soil, sand, clay, and loam. Extracts were well separated on the hydrophilic interaction liquid chromatography (HILIC) and then detected by MS/MS multiple reaction monitoring mode. The type and component of solvent mixtures were optimized to cover a wide range of polarity over all eleven amine compounds with high extraction efficiencies. Extraction parameters, such as the proportion of methanol, water and NH 4 OH, the times and the period of extraction, and volumes of extraction solution were optimized. The results indicated that a mixed solvent of methanol/water (44:53, v/v) in 3.0% NH 4 OH was the optimal formulation for extraction of all 11 analytes with high mean extraction recoveries (64.4–96.1%). Specificity and sensitivity were well improved by the good separation of 11 analytes from four-type soil matrices using these optimized HILIC parameters. This method was fully validated for each analyte in four soil matrices. The linear range of 11 analytes was 0.50/0.75–500 ng·g −1 with correlation coefficient ( R 2 ) ≥0.990, and intra/inter-day accuracies were 70.3–125% with relative standard deviation (RSD) ≤19.3%. Limit of detection (LOD) of 11 analytes ranged from 0.01 to 0.5 ng·g −1 , which was far lower than those reported in previous studies. The built method accomplishes simultaneously quantitative and trace measurement of all eleven CWC-related amine compounds within a single solvent extraction and detection. It only takes a small amount of soil samples and possesses the highest sensitivity over all previous methods. This study provides an optional recommended operating procedure for determination of CWC-related amine compounds in four typical types of complex soils during chemical weapons verification.

CAS / MDL: 105-59-9
研究领域: 分析化学 · 环境科学
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-10 · IF 14.7

Wide-energy programmable microwave plasma-ionization for high-coverage mass spectrometry analysis

Chu Fengjian,Zhao Gaosheng,Wei Wei,Shuaibu Nazifi Sani,Feng Hongru,Pan Yuanjiang,Wang Xiaozhi

Although numerous ambient ionization mass spectroscopy technologies have been developed over the past 20 years to address diverse analytical circumstances, a single-ion source technique that can handle all analyte types is still lacking. Here, a wide-energy programmable microwave plasma-ionization mass spectrometry (WPMPI-MS) system is presented, through which MS analysis can achieve high coverage of substances with various characteristics by digitally regulating the microwave energy. In addition, ionization energy can be rapidly scanned using programmable waveforms, enabling the simultaneous detection of biomolecules, heavy metals, non-polar molecules, etc., in seconds. WPMPI-MS performs well in analyzing real samples, rapidly analyzing nine toxicological standards in one drop of serum, and demonstrating good quantification and liquid chromatography coupling capability. The WPMPI-MS has also been used to detect soil extracts, solid pharmaceuticals, and landfill leachate, further demonstrating its robust analytical capabilities for real samples. The prospective uses of the technology in biological and chemical analysis are extensive, and it is anticipated to emerge as a viable alternative to commercially available ion sources.

研究领域: 分析化学 · 生物医学工程 · 环境科学
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JOURNAL OF CHROMATOGRAPHY A · 2022 · IF 4.601

Development of an online μ-matrix cartridge extraction method for fipronil extraction in contaminated soils

Ying Liu,Xinmeng Tian,Hui Xu,Ganbing Zhang

Nowadays, environment fate and behavior of pesticides in soil is still not fully understood due to the lack of standardized soil extraction method. In this work, a soil-filled micro-matrix cartridge was online combined with high performance liquid chromatography-mass spectrometry (HPLC-MS) through a six-way valve for the simultaneous extraction and determination of residual fipronil in soil. Compared with conventional extraction methods, such as hydroxypropyl-β-cyclodextrin (HPCD) extraction, shaking extraction, ultrasonic-assisted extraction (UAE), three-step extraction and matrix solid phase dispersion (MSPD), the novel, miniaturized, and integrated online micro-matrix cartridge extraction (online μ-MCE) method exhibited better performance in terms of desorption efficiency (99.4%), analysis time, solvent consumption, sensitivity, and automation. In sequential extraction, online μ-MCE could further desorb fipronil from the extracted soil with the percentage of 1.05%-58.55%. High recovery of 92.69% obtained for the ISO certificated test- soil verified the satisfactory accuracy of the method. Besides, its wide universality was also validated in three variables: 1) various pesticides-soil interactions, 2) four types of compounds (aromatic hydrocarbons, carboxylic acids, alcohols and aldehydes), and 3) three types of soils (sandy soil, silty loam and silty clay). The superior desorption capacity might be attributed to the instantaneously increased high-pressure, continuous flow dynamic desorption and short residence time. The present encouraging findings might shed light on new ways to develop a mild, highly efficient, reliable and one-fit-all extraction method toward pesticide contaminated soil.

研究领域: 环境科学 · 分析化学 · 土壤学
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ANALYTICA CHIMICA ACTA · 2021 · IF 6.558

A simple paper-based ratiometric luminescent sensor for tetracyclines using copper nanocluster-europium hybrid nanoprobes

Mengjiao Mo,Xueshen Wang,Lingyue Ye,Yaoquan Su,Yang Zhong,Lingzhi Zhao,Yunyun Zhou,Juanjuan Peng

Tetracyclines (TCs), as one of the broad-spectrum antibiotics, are widely used to treat bacterial infections. The residues of TCs in animal-origin foods and drinking water have raised safety concerns and affected the public health. Thus, there is a high demand to develop a simple and rapid method for the detection of TCs. In this work, we developed a ratiometric luminescence probe for the sensitive and visualized detection of TCs. Specifically, tannic acid-stabilized copper nanoclusters (TA-CuNCs) with blue emission at 433 nm were synthesized. The luminescence of TA-CuNCs attenuated partially by the europium ions (Eu 3+ ) due to the aggregation-induced quenching. When TCs were added to the TA-CuNCs-Eu 3+ system, the luminescence of TA-CuNCs at 433 nm can be further quenched by the inner-filter effect, and the characteristic luminescence of Eu 3+ at 617 nm emerged due to the formation of Eu 3+ -TCs complex. The ratio of the luminescence at 617 nm–433 nm increased linearly to the concentration of TCs. Additionally, we demonstrated the detection of oxytetracycline in real samples such as tap and lake water, milk, pharmaceutical industry wastewater, honey and soil extract with high recovery rate (97.25%–103.44%). Furthermore, a portable paper device is fabricated by the luminescent probe to conduct the on-site analysis of TCs.

研究领域: 分析化学 · 环境科学 · 材料科学 · 纳米技术
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