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JOURNAL OF HAZARDOUS MATERIALS · 2022 · IF 14.224

MXene−reinforced octahedral PtCu nanocages with boosted electrocatalytic performance towards endocrine disrupting pollutants sensing

Xian Liu,Like Chen,Yang Yang,Liping Xu,Junyong Sun,Tian Gan

Rational tailoring of hollow and porous bimetallic structures with excellent electrocatalytic performance is appealing yet challenging. Further, combining independent bimetallic nanoparticles with flexible two-dimensional substrate by forming stable heterocomplex is still highly desired for electrocatalysis. Herein, hierarchical PtCu alloy octahedrons with hollow interiors and nanosheet-assembled nanoshells were synthesized by a facile and efficient chemical transformation strategy using Cu 2 O as sacrificial templates. Such octahedral PtCu nanocages displayed significantly enhanced electrocatalytic activity owing to their unique hollow and porous architectures which provided easy access for analytes to the catalyst surface. Thereafter, introduction of Ti 3 C 2 T x MXene was realized via simple incubation of Ti 3 C 2 T x in solution containing the 3-aminopropyltriethoxysilane-capped PtCu, and their electrostatic interaction guaranteed the firm adsorption of PtCu nanocages on Ti 3 C 2 T x nanosheets. It turned out that the sensitivity of the hybrid sensor was remarkably improved for electrochemical monitoring of endocrine disrupting pollutants in water, exhibiting ultrawide linear ranges and sub-nanomole detection limits. The eminent electrode performance is attributed to the high specific area, fast electrochemical kinetics, decent electrical catalytic ability, and the synergistic effect between Pt, Cu, and MXene.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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JOURNAL OF HAZARDOUS MATERIALS · 2022 · IF 14.224

Split aptamer remodeling-initiated target-self-service 3D-DNA walker for ultrasensitive detection of 17β-estradiol

Shuo Qi,Xiaoze Dong,Yuhan Sun,Yin Zhang,Nuo Duan,Zhouping Wang

DNA walker machines, as one of the dynamic DNA nanodevices, have attracted extensive interest in the field of analysis due to their inherent superiority. Herein, we reported a split aptamer remodeling-initiated target-self-service 3D-DNA walker for ultrasensitive, specific, and high-signal-background ratio determination of 17β-estradiol (E2) in food samples. Two split probes (STWS-a and STWS-b) were rationally designed that can undergo structural reassembled to serve as walking strands (STWS) under the induction of the target. Meanwhile, an intact E6-DNAzyme region was formed and activated at the tail of STWS. The activated E6-DNAzyme then continuously drives the 3D-DNA walker for signal amplification and specific detection of E2. Under optimal conditions, the proposed DNA walker-based biosensor exhibited excellent linearity in the range of 1 pM to 50 nM with a low limit of detection (LOD) of 0.28 pM, and good precision (2.7%) for 11 replicate determinations of 1 nM of E2. Furthermore, the developed DNA walker-based biosensor achieved excellent sensitive analysis of E2 in the complex food matrix with recoveries of 95.6–106.5%. This newly proposed split aptamer-based strategy has the advantages of ultrasensitive, high signal-to-background ratio, and high stability. Noteworthy, the successful operation of the DNA walker initiated by the split aptamer expands the principles of DNA walker design and provides a universal signal amplification platform for trace analysis.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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NEW JOURNAL OF CHEMISTRY · 2022 ·Vol. 46 ·期 24 ·11927-11933 · IF 3.925

Preparation, characterization and application of double yolk–shell structure magnetic molecularly imprinted polymers for extraction of 17β-estradiol

Hui Lyu,Xinze Wu,Yinpeng Yang,Huaixia Chen,Xueping Dang,Xiaolan Liu

Novel double yolk–shell structure molecularly imprinted polymers were synthesized by surface polymerization with 17β-estradiol as the template, followed by chemical etching. The prepared polymers were characterized by transmission electron microscopy, nitrogen adsorption–desorption experiments, thermal gravimetric analysis and magnetic property experiments. For 17β-estradiol, the double yolk–shell structure showed a 60% improvement in the binding capacity compared to the single layer structure, and the cycle life was at least 18 times. The obtained polymers were applied as the adsorbent for magnetic solid-phase extraction (MSPE) for 17β-estradiol. Under the optimal conditions, an MSPE-HPLC method was developed for the detection of 17β-estradiol in milk powder. A wide linearity range of 0.3–300 μg kg−1 (R2 = 0.9997) for 17β-estradiol was obtained, and the limit of detection was 0.1 μg kg−1. Satisfactory recoveries ranged from 92.50% to 101.1% and relative standard deviations were lower than 6.1%. The established MSPE-HPLC method has been proven to be accurate for the analysis of 17β-estradiol in milk powder.

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ANALYTICA CHIMICA ACTA · 2022 · IF 6.911

Porous capillary monolithic column coupled with ultrahigh performance liquid chromatography-tandem mass spectrometry for fast and effective separation and determination of estrogens

Yanqun Yang,Yipeng Huang,Zhuqiang Wu,Rui Shi,Zhengyi Chen,Guihua Ruan

In this work, a porous capillary monolithic column was simply prepared by in situ thiol-alkyne click polymerization of dipentaerythritol hexakis (3-mercaptopropionate) and dimethyl dipropargylmalonate in fused-silica capillary. The capillary monolithic column shows excellent permeability, high porosity, and thoiether-rich groups, thereby, a high-efficient capacity for trace estrogens from complex samples are obtained via electron-donor-acceptor π-π interaction and hydrophobic interaction. The highest adsorption efficiency for estrogens is achieved at pH = 7.0 with a flow rate of 0.200 mL min −1 . The superior adsorption capacities of the as-prepared capillary column for eight estrogens range from 0.092 mg m −1 to 0.31 mg m −1 . A simple, reliable, and sensitive method for the determination of eight estrogens in biological and environmental samples is developed using the monolithic polymer as in-tube solid-phase microextraction coupled with ultrahigh performance liquid chromatography-tandem mass spectrometry (SPME-UPLC-MS/MS), and the total instrumental analysis time for the SPME-UPLC-MS/MS procedures was about 60 min per sample. The developed method shows a wide linear range (0.0500–5.00 μg L −1 ), and low limits of detection (5.34–9.63 ng L −1 ) for estrogens. The concentrations of estrogens in serum, urine, and pond water samples are found to be no more than 3.69, 0.741, and 1.04 μg L −1 , respectively, and the satisfying recoveries for the eight estrogens range from 80.3% to 113% with relative standard deviations ( n  = 5) of 1.5–9.4%. The established method is highly potential for extraction and analysis of ultratrace target estrogens in complex matrices, such as biological and environmental samples.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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CHROMATOGRAPHIA · 2022 ·Vol. 85 ·期 8 ·733-741 · IF 2.213

Development of an Efficient Solid-Phase Microextraction Monolithic Column for the Analysis of Estrogens in Human Urine and Serum Samples

Zhang Qianchun,Wang Yutong,Yang Bingnian,Bao Linchun,Wu Yun,Wang Xingyi

Estrogen plays a crucial role in various stages of human development and is present in the human body at trace level; therefore, an efficient strategy for the quantitative analysis of trace estrogens is required. However, this analysis is complicated by the presence of extremely complex biological matrices. To address this challenge, a novel method based on monolithic column solid-phase microextraction and ultra-high-performance liquid chromatography-tandem mass spectrometry was developed for the sensitivity analysis of six estrogens: β-estradiol, α-estradiol, 17α-ethynylestradiol, estrone, diethylstilbestrol, and hexestrol, in human urine and serum samples. The method exhibits a low limit of detection (8.6–37 ng L −1 ), with wide linear ranges (0.10–25 μg L −1 ) for each analyte and remarkable correlation coefficients ( R 2  = 0.9953–0.9995). The developed method was successfully used to detect estrogens in urine and serum samples. The six analytes were satisfactorily recovered between 76.2 and 107% with relative standard deviations ranging from 2.5 to 8.3% ( n  = 3). The results demonstrated that the developed method, based on a poly(methacrylic acid/3-acrylamidophenylboronic acid-co-ethylene glycol dimethacrylate) monolithic column, is an effective enrichment approach toward the analysis of trace estrogens in human urine and serum samples. Graphical abstract

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MOLECULES · 2022 ·Vol. 27 ·期 7 ·2353 · IF 4.927

Smart Titanium Wire Used for the Evaluation of Hydrophobic/Hydrophilic Interaction by In-Tube Solid Phase Microextraction

Yuping Zhang,Ning Wang,Zhenyu Lu,Na Chen,Chengxing Cui,Xinxin Chen

Evaluation of the hydrophobic/hydrophilic interaction individually between the sorbent and target compounds in sample pretreatment is a big challenge. Herein, a smart titanium substrate with switchable surface wettability was fabricated and selected as the sorbent for the solution. The titanium wires and meshes were fabricated by simple hydrothermal etching and chemical modification so as to construct the superhydrophilic and superhydrophobic surfaces. The micro/nano hierarchical structures of the formed TiO2nanoparticles in situ on the surface of Ti substrates exhibited the switchable surface wettability. After UV irradiation for about 15.5 h, the superhydrophobic substrates became superhydrophilic. The morphologies and element composition of the wires were observed by SEM, EDS, and XRD, and their surface wettabilities were measured using the Ti mesh by contact angle goniometer. The pristine hydrophilic wire, the resulting superhydrophilic wire, superhydrophobic wire, and the UV-irradiated superhydrophilic wire were filled into a stainless tube as the sorbent instead of the sample loop of a six-port valve for on-line in-tube solid-phase microextraction. When employed in conjunction with HPLC, four kinds of wires were comparatively applied to extract six estrogens in water samples. The optimal conditions for the preconcentration and separation of target compounds were obtained with a sample volume of 60 mL, an injection rate of 2 mL/min, a desorption time of 2 min, and a mobile phase of acetonile/water (47/53,v/v). The results showed that both the superhydrophilic wire and UV-irradiated wire had the highest extraction efficiency for the polar compounds of estrogens with the enrichment factors in the range of 20–177, while the superhydrophobic wire exhibited the highest extraction efficiency for the non-polar compounds of five polycyclic aromatic hydrocarbons (PAHs). They demonstrated that extraction efficiency was mainly dependent on the surface wettability of the sorbent and the polarity of the target compounds, which was in accordance with the molecular theory of like dissolves like.Keywords:titanium wire;superhydrophobic;superhydrophilic;in-tube solid-phase microextraction;high-performance liquid chromatography

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JOURNAL OF FLUORESCENCE · 2022 ·Vol. 32 ·期 3 ·927-936 · IF 2.525

A Significant Fluorescent Aptamer Sensor Based on Carbon Dots and Graphene Oxide for Highly Selective Detection of Progesterone

Cui Hanyue,Lu Huan,Yang Jing,Fu Yao,Huang Yan,Li Li,Ding Yaping

In this paper, a fluorescent aptamer sensor was constructed based on the carbon dots (CDs) and graphene oxide (GO). This sensor combines the excellent fluorescence performance of CDs with the high specificity of aptamer, which can detect progesterone (P 4 ) with high sensitivity and selectivity. In the absence of P 4 , the CDs-aptamer system and GO form a fluorescence resonance energy transfer process (FRET), which quenches the fluorescence of the CDs. When P 4 is added, the aptamer specifically binds to it, resulting the fluorescence of the CDs is recovered. At optimal conditions, the fluorescence intensity recovered by the CDs has a linear relationship with the concentration of P 4 in the range of 0.1–120 nM and the detection limit is 3.3 × 10 –11 M. Besides, the sensor has satisfactory detection results of P 4 in milk, indicating that constructed method has enormous potential for application in food safety.

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SENSORS AND ACTUATORS B-CHEMICAL · 2023 · IF 8.4

A ratiometric aptasensor for simultaneous determination of two estrogens based on multicolor upconversion nanoparticles

Lixia Lu,Bingchan Song,Jianwen Gao,Xinyu Shao

Different environmental estrogens (EEs) may coexist in the same foodstuff, necessitating the establishment of a simultaneous detection method. Although there are numerous studies on the detection of EEs, few was reported on the determination of two or more estrogens at the same time except HPLC . Our efforts have been made to develop a ratiometric aptasensor based on multicolor lanthanide-doped upconversion luminescence nanoparticles (UCNPs) to realize simultaneous and sensitive detection of two EEs (bisphenol A and 17β-estradiol). Three types of core-shell UCNPs with excellent luminous properties and distinct emitting colors were successfully synthesized via doping with various lanthanide ions , two of which were conjugated with specific aptamers and act as energy donors, while another one served as a reference. Because of their excellent luminescence quenching performance, ultra-thin metallic MoS 2 nanosheets were selected as the energy acceptor. Thus, a ratiometric luminescence aptasensor was established and successfully used for the simultaneous detection of two estrogens in tap water and milk samples, demonstrating its considerable practical application value.

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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Biochar nanosphere- and covalent organic framework nanosphere-functionalized titanium dioxide nanorod arrays on carbon fibers for solid-phase microextraction of organic pollutants

Mingxia Sun,Juanjuan Feng,Jiaqing Feng,Haili Sun,Yang Feng,Xiangping Ji,Chunying Li,Sen Han,Min Sun

To improve the extraction efficiency of carbon fibers (CFs) toward organic pollutants, TiO 2 nanorod arrays (NARs) were grown in situ on CFs. Subsequently, biochar nanospheres and covalent organic framework nanospheres were separately introduced to functionalize the NARs. A sequence of materials was produced by regulating the reactant concentrations and characterized using a scanning electron microscope, an X-ray photoelectron spectrometer, an X-ray diffractometer, a Raman spectrometer, and a specific surface area analyzer. The materials were then deposited into separate poly(etheretherketone) tubes for in-tube solid-phase microextraction (IT-SPME). These tubes were evaluated with different types of organic pollutants (polycyclic aromatic hydrocarbons (PAHs), estrogens, bisphenols, and phthalate esters) using a combination of high-performance liquid chromatography and IT-SPME, and they exhibited diverse extraction performance. The extraction mechanism of each material is carefully discussed, and the structure–performance relationship is also summarized based on the chemical structures and extraction properties of the materials. The most efficient extraction materials for different analytes were discovered and used to develop analytical methods. Three online methods were used to sensitively detect PAHs, estrogens, and bisphenols in real water samples, respectively. Satisfactory results were obtained, including enrichment factors up to 6784, detection limits as low as 0.001 μg L −1 , linear ranges of 0.003–15.0 μg L −1 , and relative standard deviations ranging from 0.2% to 15.2%. The results indicate that these methods have some advantages over previous material-based methods.

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FOOD CHEMISTRY · 2021 · IF 7.514

A fluorescence aptasensor based on carbon quantum dots and magnetic Fe3O4 nanoparticles for highly sensitive detection of 17β-estradiol

Qingyi Wei,Peiyao Zhang,Hongbin Pu,Da-Wen Sun

Trace amounts of 17 β -estradiol (E2) in food and the environment poses a threat to human health, which has created the demand for sensitive analytical methods to detect E2. In this study, a novel fluorescent aptasensor was developed for sensitive detection of E2 based on double-chain hybridization between carbon quantum dots-labelled with E2 aptamer (CQDs-aptamer) and Fe 3 O 4 nanoparticles modified by complementary DNA (Fe 3 O 4 -cDNA). Under the optimal conditions, the aptasensor displayed a good linear range of 10 -11 –10 -6 M for E2 with the coefficient of determination (R 2 ) of 0.996, and a low detection limit of 3.48 × 10 -12 M was obtained. Besides, the aptasensor showed high selectivity and good reproducibility for E2 detection, which was successfully applied to the sensitive detection of E2 in milk as compared with tap water and lake water with satisfactory recoveries from 85.21% to 114.80%, suggesting the great significance of this aptasensor for detecting food contaminants in the food industry.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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NEW JOURNAL OF CHEMISTRY · 2021 ·Vol. 46 ·期 2 ·808-819 · IF 3.591

Metal organic framework/chitosan/polyethylene oxide composite columnar foam as a sorbent for the enrichment and determination of estrogens in environmental aqueous solutions

Huizhong Si,Pingping He,Xuemei Wang,Lin Li,Xiaohong Hou

In this work, a metal organic framework/chitosan/polyethylene oxide composite MIL-53(Al)/CS/PEO columnar foam was successfully designed and fabricated, in which polyethylene oxide (PEO) was applied to serve as a porogen to improve the MOF loading capacity of the MIL-53(Al)/CS/PEO foam. The inherent characteristics, e.g. mechanical strength and stability of the modified foams, were also significantly improved. The MIL-53(Al)/CS/PEO columnar foam was chosen as a sorbent to develop a vortex-assisted solid phase extraction (VA-SPE) for the first time. The adsorption performance of the MIL-53(Al)/CS/PEO columnar foam was measured by choosing two typical estrogens as models to discuss the adsorption behavior. The maximum adsorption capacities of estradiol (E2) and ethinyloestradiol (EE2) are 75.2 and 42.0 μg g−1, respectively. The efficient method was then successfully applied for the extraction of trace levels of four estrogens (estrone, estradiol, estriol and ethinyloestradiol) in bulk volume environmental water, followed by high-performance liquid chromatography-fluorescence detection (HPLC-FLD). Satisfactory results of the methodology validation were obtained. Under the optimum conditions, the linear ranges were 0.02 to 40 μg L−1 with a coefficient of determination (R2) from 0.9953 to 0.9996. The method showed a lower limit of detection in the range of 0.3–6.6 ng L−1. In addition, the recoveries ranged from 73.5% to 116.7% with relative standard deviations smaller than 8.6%. The proposed columnar foam was durable, and the method employed was simple and environmentally friendly. Moreover, the foam can maintain its adsorption ability after recycling several times. The novel method proposed in this work could provide a simple and efficient sample preparation and has great application potential for sample pretreatment in a bulk mass aqueous sample.

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FOOD CHEMISTRY · 2023 · IF 8.8

Membrane–protected magnetic covalent organic framework for efficient extraction of estrogens in dairy products

Cheng Yang,Zheng–Lian Mo,Qiu–Fang Zhang,Jin–Jie Xu,Xiao–Fang Shen,Yue–Hong Pang

The presence of estrogens residues in dairy products is a growing concern due to their potential health risk. Herein, in this study, we have developed a membrane–protected magnetic solid–phase extraction (MP–MSPE) method that utilized a magnetic adsorbent (Fe 3 O 4 @COF–LZU1) with in–situ growth for the efficient extraction of estrone (E1), 17β–estradiol (E2), and estriol (E3). When combined with HPLC–FLD, this method allows for the efficient detection of estrogens in dairy products. The stability of the MP–MSPE was improved by the presence of a dialysis membrane, which remained a high extraction efficiency (90 %) even after ten reuse cycles. The hydrogen bonding, π–π interactions and pore size effect contribute to the excellent adsorption of three estrogens onto Fe 3 O 4 @COF–LZU1. Under optimal conditions, the method exhibits a low detection limit (0.01–0.15 μg L −1 ), wide linear range (0.1–800 μg L −1 ), and favorable recoveries (77.3 %–109.4 %) at three concentration levels (10, 50 and 100 μg L −1 ). This proposed method is characterized by its simplicity, high efficiency and eco–friendliness, making it a promising approach for extracting estrogens from dairy products.

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