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ANALYTICA CHIMICA ACTA · 2023 · IF 6.2

Fluorescent sensor based on solid-phase extraction with negligible depletion: A proof-of-concept study with amines as analytes

Miao Zhang,Rana Dalapati,Jiangfan Shi,Chenglong Liao,Qingyun Tian,Chuanyi Wang,Xiaomei Yang,Shuai Chen,Marc D. Porter,Ling Zang

This paper describes the development and proof-of-concept testing of an easy-to-use trace analysis technique, namely F-SPE, by coupling fluorescent sensor with solid phase extraction (SPE). F-SPE is a two-step methodology that concentrates an analyte from a liquid sample onto a fluorophore-modified membrane and measures the amount of analyte from the extent the extracted analyte quenches the emission of the fluorophore. By applying the principle of negligible depletion (ND) intrinsic to SPE , the procedure of F-SPE for analyzing a sample can be markedly simplified while maintaining the ability to detect analytes at low limits of detection (LOD). The merits of this approach are demonstrated by impregnating a SPE membrane with a perylene diimide (PDI) fluorophore, N,N′-di(nonyldecyl)-perylene-3,4,9,10-tetracarboxylic diimide (C9/9-PDI), for the low-level detection of organic amines (e.g., aniline) and amine-containing drugs (e.g., Kanamycin). The sensing mechanism is based on the donor-acceptor quenching of PDI by amines, which, when coupled with the concentrative nature of SPE, yields LODs for aniline and Kanamycin of 67 nM (∼6 ppb) and 32 nM (∼16 ppb), respectively.

研究领域: 分析化学 · 环境科学 · 材料科学
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MICROCHEMICAL JOURNAL · 2023 · IF 4.8

Electrochemical aptasensor based on 3D graphene aerogel for prostate specific antigen detection

Tao Hu,Zeyang Bai,Di Wang,Ying Bai,Xiao Li,Zhonghua Ni

Prostatic cancer threatens the lives and health of numerous male patients all over the world. As a single-chain glycoprotein, prostate specific antigen (PSA) can be used to perform prostate cancer screening. At present, there are still problems such as time-consuming and low sensitivity in hospital detection. At the same time, electrochemical immunosensor technology has received a lot of attention due to its benefits, including high sensitivity, good selectivity, low usage and cost, and so on. Electrocatalysts are typically used to build electrochemical immunosensors for signal amplification in the recent years to realize sensitive detection of cancer biomarkers such as PSA. In recent years, three-dimensional nanomaterials have been widely used in the study of electrocatalysts, but the study of the sensitivity for PSA detection is still very scarce. The present work reported the application of a 3D graphene aerogel(GA)/AuNPs/Nafion electrochemical platform for highly sensitive PSA quantification. The electrochemical immunosensor has been designed by immobilizing aptamers on the screen-printed electrode (SPE) surface modified by GA/AuNPs/Nafion. Scanning electron microscopy (SEM), Raman spectra, and electrochemical characterization demonstrated the successful combination of GA/AuNPs/Nafion/SPE. Based on electrochemical impedance spectroscopy (EIS), the proposed immunosensor has demonstrated excellent electrochemical performance, exhibiting sensitive and stable responses for electrochemical detection of PSA ranging from 0.05 to 50 ng∙mL −1 with a limit of detection (LOD) of 0.0306 ng∙mL −1 . This study has great potential application in PSA detection and provides a valuable reference for point-of-care testing (POCT) of prostate cancer.

研究领域: 生物化学 · 分析化学 · 生物传感器 · 癌症研究 · 材料科学 · 电化学
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Food Analytical Methods · 2017 ·Vol. 10 ·期 10 ·3434-3442 · IF 2.038

SPE-UHPLC-DAD Method for the Simultaneous Determination of Three Flavonoids in Grape Juice by Using Bis(tetraoxacalix[2]arene[2]triazine)-Modified Silica as Sorbent

Hu Kai,Deng Zhifen,Li Sui,Wu Mingxia,Liu Wei,Zhang Shusheng

In this study, bis(tetraoxacalix[2]arene[2]triazine) modified silica gel was successfully prepared and used as an efficient sorbent for solid-phase extraction. Coupled with ultra-high pressure liquid chromatography (UHPLC), the extraction performance of the sorbent was evaluated by using three flavonoids as model analytes. Main parameters, which affecting extraction efficiency were carefully optimized. The results showed that multiple intermolecular interactions were involved in the sample pretreatment procedure, including π–π, hydrophobic and hydrogen bonding interactions. Under the optimal conditions, the proposed method was applied for the analysis of three flavonoids in grape juice. Satisfactory linear ranges for flavonoids were obtained in the range of 5–200 ng mL −1 for quercetin, 1–200 ng mL −1 for luteolin, and 2–200 ng mL −1 for kaempferol, with good correlation coefficients (>0.9996). Limits of detection (LODs) were in the range of 0.5–2 ng mL −1 , and the LOQs were between 1 and 5 ng mL −1 . The recovery values of spiked grape juice ranged from 97 to 106% with relative standard deviations (RSDs) less than 4.7% ( n  = 3). This method exhibited the advantages of simplicity, rapidity, and low solvent consumption, and was promising for the separation and determination of flavonoids in grape juice and other matrixes.

研究领域: 分析化学 · 食品科学
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CHROMATOGRAPHIA · 2012 ·Vol. 75 ·期 15 ·883-892 · IF 1.195

Automated On-Line SPE/Multi-Stage Column-Switching and Benzoic Acid-Based QAMS/RODWs-HPLC for Oral Pharmacokinetics of Syringic Acid and Salicylic Acid in Rats

Zhou Wei,Zhang Yanhai,Ning Suli,Li Yan,Ye Mingli,Yu Yingjia,Duan Gengli

Automated on-line SPE/multi-stage column-switching and benzoic acid-based quantitative analysis of multi-components by single-marker/respective optimal detection wavelengths-high performance liquid chromatography (QAMS/RODWs-HPLC) as a novel analysis model was reported in the study; it obtained simple, effective, very low-cost, sensitive and reliable characteristics. This method has been set up for direct analysis of syringic acid, benzoic acid, and salicylic acid in rat plasma, and its application to the pharmacokinetic study of syringic acid and salicylic acid in rats. The chromatographic separation was performed on two C18 columns with the elution of methanol and 0.5 % formic acid aqueous solution in two pump systems, detection wavelengths of 230, 236, and 275 nm, 500-μL injection volume. Their linear ranges were between 0.008 and 166.7 μg mL −1 with correlation coefficient of 0.9977–0.9997. Benzoic acid-based QAMS/RODWs-HPLC was also compared with other two quantitative analysis methods (external standard method of RODWs-HPLC, internal standard method of RODWs-HPLC) based on pharmacokinetic data; the similarities of three analytical methods in accordance with separately obtained concentrations of syringic acid and salicylic acid in rats were 0.9997–0.9999 by the cosine value method of vectorial angle. The pharmacokinetics of syringic acid and salicylic acid were simultaneously studied in SD rats following 30 mg kg −1 intragastric administration, and their pharmacokinetic parameters were also estimated. This method was successfully applied to determination of syringic acid and salicylic acid in rat plasma samples and their oral pharmacokinetics in rats.

CAS / MDL: 530-57-4 69-72-7
研究领域: 分析化学 · 药理学 · 生物医学
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Journal of Analytical Methods in Chemistry · 2017 · IF 1.801

SPE-UHPLC-FLD Method for the Simultaneous Determination of Five Anthraquinones in Human Urine Using Mixed-Mode Bis(tetraoxacalix[2]arene[2]triazine) Modified Silica as Sorbent

Kai Hu,Yonghui Qiao,Zhifen Deng,Mingxia Wu,Wei Liu

The five anthraquinones compounds (including aloe-emodin, emodin, physcion, chrysophanol, and rhein) are regarded as the main effective ingredients in rhubarb (Dahuang in Chinese, one of the commonly used Chinese herbal medicines). In this work, a simple and effective solid phase extraction (SPE) method based on bis(tetraoxacalix[2]arene[2]triazine) modified silica gel as adsorbent was developed. Coupled with UHPLC-FLD, the developed method was successfully applied for the measuring of main anthraquinones in human urine after oral administration of the extracts of rhubarb. To obtain the highest recoveries of the five anthraquinones in the SPE process, the main parameters which may affect extraction efficiency were optimized. The optimized sorbent amount, sample loading pH, sample loading rate, washing solution, and eluent condition were obtained. The developed method showed good linearity in 0.012–1.800 μg mL−1 for the five anthraquinones with correlation coefficients more than 0.9993. The investigated LOD values ranged from 3.9 to 5.7 ng mL−1, while the LOQs were between 12.0 and 18.2 ng mL−1. The recoveries of the method were also investigated, which were in the range of 94.8–106.6%. The application of the mixed-mode SPE materials in the proposed method was feasible and simple, and suitable for the enrichment of anthraquinones in urine samples.

研究领域: 中药分析 · 色谱技术 · 药物代谢研究
✓ 已验证 DOI PubMed 高影响因子
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ANALYTICA CHIMICA ACTA · 2024 · IF 5.7

For the occurrence of PPCPs from source to tap: A novel approach modified in terms of sample preservation and SPE cartridge to monitor PPCPs in our water supply

Yu Wang,Qianzhan Yang,Huadong Zhang,Zhenghong Wang,Ailin Wu,Yun Luo,Qianru Zhou

Background The ongoing infusion of pharmaceutical and personal care products (PPCPs) into ecosystems sustains a perpetual life cycle and leads to multi-generational exposures. Limited understanding of their environmental impact and their intrinsic ability to induce physiological effect in humans, even at low doses, pose great risks to human health. Few scholarly works have conducted systematic research into the occurrence of PPCPs within potable water systems. Concurrently, the associated monitoring techniques have not been comprehensively examined with regards to the specific nature of drinking water, namely whether the significant presence of disinfectants may influence the detection of PPCPs. Results A modified approach in terms of detailed investigation of sample preservation and optimization of an in-lab fabricated solid phase extraction (SPE) cartridge filled with DVB-VP and PS-DVB sorbent was proposed. Favorable methodological parameters were achieved, with correlation coefficients spanning from 0.9866 to 0.9998. The LODs of the PPCPs fluctuated from 0.001 to 2 μg L −1 , while the LOQs varied from 0.002 to 5 μg L −1 . The analysis of spiked samples disclosed a methodological precision of 2.31–9.86 % and a recovery of 52.4–119 %. We utilized the established method for analyzing 14 water samples of three categories (source water, finished water and tap water) from five centralized water supply plants. A total of 24 categories encompassing 72 PPCPs were detected, with the concentrations of PPCPs manifested a marked decrease from source water to finished water and finally to tap water. Significance Our research meticulously examined the enhancement and purification effects of widely used commercial SPE cartridges and suggested the use of in-lab fabricated SPE cartridges packed with DVB-VP and PS-DVB adsorbents. We also conducted a systematic evaluation of the need to incorporate ascorbic acid and sodium thiosulfate as preservatives for PPCP measurement, in consideration of the unique characteristics of drinking water matrices, specifically, the significant concentration levels of disinfectants. Furthermore, the proposed method was effectively employed to study the presence of PPCPs in source water, finished water, and tap water collected from centralized water supply plants.

研究领域: 环境科学 · 分析化学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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JOURNAL OF AOAC INTERNATIONAL · 2025 · IF 1.7

Polydopamine-Coated Magnetic Molecularly Imprinted Polymers as a Dispersive SPE Adsorbent for Selective Recognition and Enrichment of Basic Orange 2 in Food Matrices with High-Performance Liquid Chromatography Analysis

Hu Meihua

BackgroundBasic orange 2, as an industial dye, exhibits severe effects to human health and has been forbidden to use as food additives in many countries. The practical use of common pretreatment process for basic orange 2 in food might be limited owing to time consuming, high consumption of solvents and weak selectivity. Therefore, the aim of this study was to validate a pre-treatment technology for basic orange 2 based on simplicity, being rapid, good selectivity, high sensitivity and inexpensiveness to ensure the tongue safety for people.ObjectivesTo develop a strategy for the extraction and enrichment of basic orange 2 in food matrices by the specific magnetic molecularly imprinted polymers prior to the determination by HPLC.MethodsThe polymers with basic orange 2 as the template were deposited on the surface of ferroferric oxide nanoparticles (Fe3O4@PDA MIPs) through the self-assembly of dopamine in the weak alkaline solution. The Fe3O4@PDA MIPs as a disperse SPE sorbent were used for extracting and detecting basic orange 2 using HPLC. Parameters influencing extracting efficiencies were optimized, including the mass of MIPs, pH value, time for ultrasonication, elution solvent and volume.ResultsUnder optimal experimental conditions, the detection linearity of basic orange 2 was in the range of 0.04–1.0 μg/mL with correlation coefficient of 0.9991 and the limit of detection (LOD) of 5.8 ng/mL. The recoveries from spiked samples were 73.3%-90% with RSD 3.1%-8.1% in food samples. Notably, the magnetic MIPs showed an excellent reusability during 3 times extraction procedures.ConclusionThe Fe3O4@PDA MIPs prepared have great potential for purification and enrichment of basic orange 2 prior to its determination by HPLC in dried beancurd stick, yellow fish, chili powder, drinks and wine.HighlightsThe magnetic MIPs developed show good adsorption performance for basic orange 2 with a very low detection, and excellent reusability. The assay was applied to detect basic orange 2 in food samples successfully.

CAS / MDL: 77-86-1
研究领域: 食品科学 · 分析化学
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TALANTA · 2013 · IF 3.498

Preparation of a hollow porous molecularly imprinted polymer using tetrabromobisphenol A as a dummy template and its application as SPE sorbent for determination of bisphenol A in tap water

Jin Li,Xuebin Zhang,Yuxin Liu,Hongwu Tong,Yeping Xu,Shaomin Liu

In this paper, a highly selective sample cleanup procedure combing dummy molecular imprinting and solid-phase extraction (DMIP–SPE) was developed for the isolation and determination of bisphenol A (BPA) in tap water. The novel hollow porous dummy molecularly imprinted polymer (HPDMIP) was prepared adopting a sacrificial support approach, using tetrabromobisphenol A (TBBPA), whose structure was similar to that of BPA, as the dummy template and mesoporous MCM-48 nanospheres as the support. Owing to a very short distance between the binding sites and the surface, a large surface area and a good steric structure to match its imprint molecules, the maximum adsorption capacities ( Q max ) of the dummy-imprinted and non-imprinted sorbents for BPA were as high as 445 and 340   μmol   g –1 , respectively, and the adsorption reached about 73% of Q max in 10   min. Meanwhile, a method was developed for the determination of BPA using HPDMIP as a solid-phase extraction enrichment sorbent coupled with HPLC . Under the optimum experimental conditions, HPDMIP exhibited satisfactory results in the enrichment and determination of BPA in tap water with a recovery rate of 95–105%, and relative standard deviations of below 6%, and it can achieve a limit of detection as low as 3   ng   mL −1 . The developed extraction protocol eliminated the effect of template leakage on quantitative analysis and could be applied for the determination of BPA in complicated functional samples.

研究领域: 环境科学 · 分析化学
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Food Analytical Methods · 2021 ·Vol. 14 ·期 8 ·1577-1589 · IF 3.366

Preparation and Application of β-Cyclodextrin Functionalised Graphene Oxide-Grafted Silica Sorbents for Solid-Phase Extraction (SPE) of Polycyclic Aromatic Hydrocarbons from Fried Food Using a Box-Behnken Design

Wang Na,Lu Yanmin,Cui Bo

A β-cyclodextrin functionalised graphene oxide-grafted silica (β-CD@GO/SiO 2 ) sorbent was synthesised and used as a solid-phase extraction (SPE) sorbent for the extraction of trace polycyclic aromatic hydrocarbons (PAHs) from fried food extract. The prepared β-CD@GO/SiO 2 was characterised using Fourier transform infrared spectrometry (FT-IR) and elemental analysis (EA). Compared with graphene oxide-grafted silica (GO/SiO 2 ), the β-CD@GO/SiO 2 had better extraction selectivity for 4- to 5-ring PAHs, which benefitted from the size complementarity between β-CD@GO/SiO 2 and PAHs arising from the introduction of β-CD. In addition, the results of selective extraction were confirmed by theoretical calculation. Following single-factor experiments, response surface methodology (RSM) was used to optimise extraction and elution parameters. Under the optimal conditions, a method was developed to combine the SPE technique with high-performance liquid chromatography (HPLC). Linear ranges of 1–100 and 0.3–100 μg L −1 with correlation coefficients ( R 2 ) ranging from 0.9980 to 0.9995 were obtained. Limits of detection were in the range of 0.1–0.3 μg L −1 . The intra-day and inter-day precisions were less than 3.9 and 5.5%, respectively. In addition, the method was successfully applied to determine PAHs in fried food with satisfactory spiked recoveries.

研究领域: 分析化学 · 食品安全
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

A ketone-containing all-solid-state polymer electrolyte with rapid Li-ion conduction for lithium metal batteries

Pingping Chen,Qinghui Zeng,Qingyuan Li,Ruihua Zhao,Zhenfeng Li,Xin Wen,Wen Wen,Yu Liu,Anqi Chen,Zengxi Li,Xiangfeng Liu,Liaoyun Zhang

Solid-state polymer electrolytes (SPEs) have gained considerable attention in the application of all-solid-state lithium batteries (ASSLBs), but the low ionic conductivity at room temperature and inferior interfacial compatibility largely drag the practical development of SPEs. Herein, a ketone-containing poly(allyl acetoacetate) (PAAA) based polymer electrolyte is designed and prepared for the first time. The structure of ester and ketone groups provides PAAA polymers with not only strong dissociation of lithium salts but also weak coordination interactions with Li + ions. Thus the prepared PAAA polymer electrolytes show excellent ion conductive behavior with ionic conductivity as high as 1.1 × 10 -4  S cm −1 at 30 °C. Moreover, the PAAA polymer electrolytes still maintain superior viscoelasticity without compromising mechanical integrity. When assembling cells, the reduction-tolerant poly(ethylene oxide) (PEO) polymer electrolytes are employed as interlayers between the PAAA SPEs and lithium electrodes in order to improve interfacial stability. As a result, the hierarchical polymer electrolytes possess wide electrochemical window above 4.8 V, thus matching well with LiFePO 4 or Li 1.2 Ni 0.2 Mn 0.6 O 2 high-voltage cathode. The hierarchical structure does not affect interfacial contact, and the Li/PEO-PAAA-PEO/Li cells show low interfacial resistance and stable striping/plating behavior for at least 500 h at 0.2 mA cm −2 and 60 °C. This study enriches carbonyl-based polymer electrolytes by allying ketone with ester groups, and provides guidance for designing novel high-performance polymer electrolytes for practical application.

研究领域: 材料科学 · 电化学 · 电池技术
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Analytical Methods · 2021 ·Vol. 13 ·期 38 ·4442-4451 · IF 2.896

A simple unlabeled human chorionic gonadotropin biosensor based on a peptide aptamer

Huanhuan Li,Tongji Cai,Yi Ren,Jing Huang,Hanbing Jiang,Yucui Hou,Chunhua Tang,Jie Yang,Jia Zhao,Peng Yu

As an essential biochemical indicator in the fields of pregnancy and oncology, human chorionic gonadotropin (HCG) can be evaluated using colloidal gold immunochromatographic paper and quantified using a biochemical analyzer based on the principle of the antibody sandwich method. In view of the inaccuracy of the former and the complication of the latter, this study constructed an accurate, sensitive and simple unlabeled biosensor based on peptide aptamer CGGGPPLRINRHILTR for HCG detection. Molecular Operating Environment (MOE) was used to simulate the aptamer and protein docking, and western blot (WB) was used to verify the binding effect and ratio. The peptide aptamer was characterized and was then reduced with tris-(2-carboxyethyl)-phosphine hydrochloride (TCEP). After electrochemical deposition of chloroauric acid on the screen-printed electrode (SPE), the aptamer was self-assembled on the electrode surface under optimal conditions. The active site of the electrode surface was blocked with 6-mercapto-1-hexanol (MCH) and BSA. The electrochemical impedance spectrum (EIS) was used to quantify HCG in the matrix. Showing a good linear relationship in the range of 5–1500 mIU mL−1, with a detection limit of 1 mIU mL−1, the biosensor remained stable at room temperature for 14 days. Because of its small size, stability, sensitivity and accuracy, this biosensor has great potential to become a portable diagnostic device for HCG.

研究领域: 生物化学 · 生物传感器 · 分析化学 · 妊娠诊断 · 肿瘤学
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JOURNAL OF CHROMATOGRAPHY A · 2019 · IF 3.858

Enhancement of liquid chromatography-ion trap mass spectrometry analysis of 4(5)-methylimidazole in biscuits through derivatization with dansyl chloride

Chunjian Wu,Li Wang,He Li,Shujuan Yu

The presence of potential carcinogen 4(5)-Methylimidazole (4-MeI) in foods causes much concern, stressing the need of a sensitive determination means. Here, we proposed a high-sensitivity method to determine 4-MeI in biscuits using dansyl chloride derivatization and disperse liquid-liquid micro-extraction (DLLME) followed by a liquid chromatography-ion trap mass spectrometry (LC-IT-MS) analysis. This developed method was subsequently compared to the solid phase extraction combining with liquid chromatography-triple quadrupole mass spectrometry (SPE-LC-QqQ-MS) method. The optimized derivatization conditions were 30 °C and 10 min. Results suggested that the column retention time (RT) was significantly extended, and the MS signal response of 4-MeI-dansyl derivative was also amplified. The developed DLLME-LC-IT-MS method in 4-MeI determination provided satisfactory linearity in a range of 0.5–300 ng/mL (R 2 > 0.9991), inter-day accuracy (87-102%) and precision (%RSD ≤ 13.6%) with the quantification limit of 0.2 ng/mL, which obtained similar results comparing to the conventional SPE-LC-QqQ-MS method.

研究领域: 分析化学 · 食品科学 · 质谱分析
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