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Pergamon Press
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Pergamon Press

0039-9140

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    A dual-mode strategy combining SERS with MALDI FTICR MS based on core-shell silver nanoparticles for dye identification and semi-quantification in unearthed silks from Tang Dynasty

    Guan M.Wei L.Liu H.Qu L....
    5页
    查看更多>>摘要:? 2022 Elsevier B.V.Silk, as one of the representative artifacts of China, profoundly affects the communication between eastern and western civilizations, and dyes, as the color support of silks, reflected crucial historical, cultural and technological information. Surface enhanced Raman spectroscopy (SERS) characterized by vibrational information has been extensively employed in dye analysis. However, since natural plants with complex coloring compositions in ancient China were broadly applied in dying textiles, the existing SERS methods often misinterpret results in dye analysis. Besides, semi-quantification of each component was of great difficulty by SERS, limiting the exquisite comparative analyses of different historical samples. For the first time, a dual-mode strategy combining SERS with high mass resolution MALDI FTICR MS was developed in virtue of core-shell silver nanoparticles (AgNPs@PDA), which realized the precise identification and semi-quantification of complex dye mixtures, thus significantly improving the accuracy and applicability of traditional SERS method. Four typical dye components (alizarin, purpurin, berberine and indigo) have been identified and semi-quantified in unearthed dyed silks from Tang Dynasty based on the method. More interestingly, multiple dye components with different contents and their ratio could be precisely determined, which might help in further investigating their dyeing techniques. This dual-mode strategy represents a promising tool for providing solid support for cognition, evaluation and restoration of textile objects in museums and conservation centers.

    Towards intelligent packaging: BCP-EVOH@ optode for milk freshness measurement

    Magnaghi L.R.Zanoni C.Alberti G.Quadrelli P....
    5页
    查看更多>>摘要:? 2022 Elsevier B.V.Intelligent packaging represents an emerging trend in the food industry, especially for highly perishable foods like milk and dairy products. Despite the apparent simplicity, miniaturized BCP-EVOH@ sensor, made of bromocresol purple (BCP) covalently bound to ethylene-vinyl alcohol (EVOH) copolymer, meets the goal of milk freshness monitoring during chilled storage, allowing both naked-eye evaluation and chemometric-assisted spoilage modelling and measurements.

    Digital-resolution and highly sensitive detection of multiple exosomal small RNAs by DNA toehold probe-based photonic resonator absorption microscopy

    Villanueva A.Zhao B.Cunningham B.T.Wang W....
    5页
    查看更多>>摘要:? 2022 Elsevier B.V.Small noncoding RNAs (snRNA) have been emerging as promising diagnostic biomarkers for detecting early stage cancer. Currently existing methods for snRNA detection, including northern blot, reverse transcription-polymerase chain reaction, microarrays and RNA-Seq, are limited to time-consuming, low sensitivity, expensive instrumentation or complex analysis of data. Herein, we present a rapid quantitative analysis of multiple liver cancer-associated exosomal snRNA by a nucleic acid toehold probe-based photonic resonator absorption microscopy (PRAM) assay, with digital resolution and high sensitivity. The assay relies on the use of three toehold probe-encoded gold nanoparticles (AuNPs) and addressable photonic crystal (PC) sensing chips. The presence of target snRNA will initiate toehold-mediated strand displacement reactions that trigger the capture of gold particles onto the PC surface, which is subsequently imaged by PRAM for digital counting of detected snRNA molecules. We achieved highly sensitive and selective detection of three snRNA targets in buffer with a 30 min assay protocol, with detection limits of 4.56 fM, 4.68 fM and 0.69 pM. Having confirmed our assay's performance for detection of snRNA targets spiked into exosomal RNA extracts, we demonstrated its capability for quantitative detection of the same targets from patient blood plasma samples. The approach offers a rapid, simple workflow that operates at room temperature with a single step without enzymatic amplification, while the detection instrument can be implemented as a low-cost portable system for point of care environments.

    A miniaturized, low-cost lens tube based laser-induced fluorescence detection system for automated microfluidic analysis of primary amines

    Duca Z.A.Speller N.C.Cato M.E.Morbioli G.G....
    5页
    查看更多>>摘要:? 2022In situ analyses are essential to ascertain potential past or present habitability in celestial bodies. One technique that provides the sensitivity and miniaturization needed to successfully detect trace organics in the outer Solar System is laser-induced fluorescence (LIF) detection, which, when coupled with microfluidic systems, provides a powerful wet chemistry platform that can meet the size and resource consumption constraints of a remote analysis mission. Herein, a portable LIF detection module (44-mm long, 18-mm wide) was prototyped and utilized to quantify bulk organics in a liquid sample via manual and automated analysis utilizing a programmable microfluidic architecture. The experimental limit of detection (LOD) for primary amines was 11.8 μM. A sample (Y31B) collected from the Atacama Desert in Yungay, Chile, was analyzed manually and found to contain 300 ± 50 μM of bulk primary amine organics, while the automated microfluidic protocol found the sample to contain 289 ± 4 μM of primary amines. Automated analyses showed no statistically significant differences when compared to the manual analyses (t-test, C.I. 95%). Our results demonstrate that the coupling of programmable microfluidic devices with a custom lens tube-based LIF detector enables automated analysis of primary amines using a protocol appropriate for remote analyses. This technique is an invaluable tool for in situ analysis applications in distant, resource-restricted environments.

    Impedimetric detection of miRNA biomarkers using paper-based electrodes modified with bulk crystals or nanosheets of molybdenum disulfide

    Yarali E.Eksin E.Erdem A.Torul H....
    5页
    查看更多>>摘要:? 2022 Elsevier B.V.Paper-based electrodes modified with molybdenum disulfide (MoS2) in the form of bulk crystals or exfoliated nanosheets were developed and used as a biosensing platform for the impedimetric detection of miRNAs (miRNA-155 and miRNA-21) related to early diagnosis of lung cancer. For this purpose, MoS2 crystals or nanosheets were used for the modification of the working electrode area of paper-based platform for the first time in this study. The proposed assay offers sensitive and selective detection of microRNAs by electrochemical impedance spectroscopy (EIS) technique. The entire assay, both the electrode modification and the miRNA detection being completed in 30 min and a single sample droplet (5 μL) was enough to cover working electrode area which enabled analysis in low sample volumes. The limits of detection (LOD) for miRNA-21 and miRNA-155 were calculated both in buffer and fetal bovine serum media. It is found that the LOD is varying between 1 and 200 ng/mL. In comparison to nanosheets, a larger electroactive surface area was obtained with bulk MoS2 resulting in lower LOD values on miRNA detection. The paper-based electrodes showed high specificity towards their target sequences. Moreover, they effectively discriminated single base mismatched non-target sequences. The advantages of these MoS2 paper based electrodes include high sensitivity, and low-cost provide great potential for improved monitoring of miRNA biomarkers even in artificial serum media.

    A high-throughput, cheap, and green method for determination of ethanol in cacha?a and vodka using 96-well-plate images

    Filgueiras M.F.de Oliveira Lima B.Borges E.M.
    5页
    查看更多>>摘要:? 2022A high-throughput method for the determination of ethanol in vodka and cacha?a using 96-well-plate digital images was proposed and validated. The standard method consists of beverage distillation, measuring its density using a pycnometer, and converting it into ethanol content. It is simple, but it is time-consuming and susceptive to error. The proposed method exploits the suppression of phenolphthalein ionization by ethanol in an alkaline solution and the fading of the pink solution was converted into ethanol content. It consists in mixing 1 mL of sample with 0.1 mL of an alkaline phenolphthalein solution. 96-well-plate images were acquired using a desktop scanner. Red, green, and blue (RGB) values from the 96 wells were automatically extracted using ReadPlate (ImageJ plugin). Then, RGB values were exported to a spreadsheet that converted these values into analytical signals and calculated the ethanol content in beverages. The ethanol content of cacha?as and vodkas was 33–45% (v/v) and it was also the linear range of the proposed method. The method's precision was evaluated using relative standard deviation (RSD). Five cacha?as and three vodkas were analyzed. Each beverage was analyzed six times on the same day (intra-day repeatability) and three consecutive days (inter-day repeatability) by three different analysts (inter-analyst repeatability). The intra-day repeatability average was 1.7% (1.2–2.2% range), the intra-day repeatability average was 2.6% (1.9–3.5% range), and the inter-analyst repeatability average was 4% (2.6–6.2% range). Accuracy was evaluated by comparing the proposed method with the standard method using a percent error and a paired t-test. The average percent error was 1.9%, in the paired t-test, the p-value average value was 0.25. The proposed method can analyze 12 samples in 30 min, whereas the standard method spends around 1 h on each sample. Thus, the proposed method provides high-throughput compared with the standard method.

    A controlled recognizing and releasing glycoprotein based on temperature-responsive phenylboronic microgels for colorimetric analysis of complex samples

    Li G.Xiao X.Su R.Xia L....
    5页
    查看更多>>摘要:? 2022 Elsevier B.V.It is challenging to capture glycoprotein from complicated samples with both high specificity and high recovery. Herein, we synthesized temperature-responsive poly (N-isopropylacrylamide-4-vinylbenzeneboronic acid) (PNIPAM-VPBA) microgels having enhanced affinity capability towards glycoprotein, resulting signal amplification in colorimetric analysis subsequently. Through temperature control, the target glycoprotein can be captured and released by the reported microgels unbiasedly. The microgels fabricated were characterized in terms of particle size, phase transition temperature, and toxicity. It was revealed that obvious changes in the particle diameter ranged from 600 to 323 nm between 25 °C and 55 °C, the volume transition temperature was close to human physiological temperature, and low toxicity towards HeLa cells after 24 h incubation. Using glucose oxidase as a model target, the microgels were applied as adsorbent materials for preconcentration of glucose oxidase, resulting 22-fold signal enhancement and a limit of detection (LOD) as low as 16.7 U/L. In beer sample analysis, satisfied recoveries of 78.7%–101.6% with the relative standard deviations (RSDs) less than 7.2% was observed. Subsequently, the microgels were combined with enzyme-linked immunosorbent assay (ELISA) for alpha fetoprotein (AFP) determination, by immobilizing horseradish peroxidase (HRP) and anti-AFP antibodies on the surface of microgels. A meaningful low concentration range of 2.5 × 10?2 to 1.0 μg/L was obtained for AFP detection using the microgels based colorimetric method with a LOD of 8.4 ng/L. In human serum sample analysis, good accuracy was achieved from method comparing with commercial ELISA kit, satisfied recoveries of 86.1%–96.4% with the RSDs less than 6.0% was observed. The proposed PNIPAM-VPBA microgels have great potential applications in the fields of food and clinical analysis.

    Sr-Nd-Hf isotopic analysis of reference materials and natural and anthropogenic particulate matter sources: Implications for accurately tracing North African dust in complex urban atmospheres

    Prospero J.Das S.Chellam S.Miller B.V....
    5页
    查看更多>>摘要:? 2022 Elsevier B.V.We present novel chemical separation protocols for isotopic analysis of low mass aliquots (0.3 mg and 25 mg) of several reference materials and real-world samples of relevance to urban airborne particulate matter (PM) investigations. A high-yielding gravity flow column chromatography scheme was developed for facile and quantitative separation of Sr, Nd, and Hf prior to multi collector – inductively coupled plasma – mass spectrometry (MC-ICP-MS). Because we are interested in isolating and accurately quantitating individual anthropogenic and natural aerosol sources in complex industrial/metropolitan atmospheric environments, laboratory protocols were optimized using National Institute of Standards and Technology Standard Reference Material (SRM) 1648a (urban atmospheric PM), SRM 1633b (coal fly ash), and European Commission standards BCR-723 (vehicular road dust), and BCR-2 (basalt rock standard). Sr, Nd, and Hf procedural blanks from column chromatography were low (averaging only 37 pg, 17 pg, 11 pg, respectively) and recoveries were high (averaging 95%, 82%, and 92%, respectively). A volume-adjustment protocol was established using isotope reference solutions SRM 987 (SrCO3), JNdi (Nd2O3), and in-house Hf standards to dilute the dried samples prior to MC-ICP-MS based on projected uncertainties for low sample masses. 87Sr/86Sr, 143Nd/144Nd, and 176Hf/177Hf isotopic ratios in SRM 1648a, BCR-723, and SRM 1633b are reported for the first time that can serve as provisional reference values. The novel method was used to characterize isotopic ratios and elemental abundances in two anthropogenic urban aerosol sources, namely motor vehicles and petroleum refining using airborne fine PM collected in a vehicular tunnel and fluidized-bed catalytic cracking catalysts, respectively. Two other important mineral-rich urban PM sources, namely soil (i.e., resuspended crustal material) and concrete/cement dust (i.e., construction activity) were also characterized. These are the first isotopic measurements in these environmental compartments and were compared with literature data for long-range transported North African dust, which is a prominent summertime PM source in urban regions in southeastern United States. We demonstrate the capability of coupled Sr-Nd-Hf isotopes to uniquely trace different mineral dust sources with overlapping elemental composition (Sahara-Sahel region, local soil, and concrete/cement) and accurately isolate various urban PM sources demonstrating the superiority of isotopic markers over elemental tracers.

    Design and fabrication of an integrated 3D dynamic multicellular liver-on-a-chip and its application in hepatotoxicity screening

    Luo G.-A.Xie Y.-Y.Ma L.-D.Wang Y.-M....
    5页
    查看更多>>摘要:? 2022 Elsevier B.V.Nowadays, major methods of in vitro hepatotoxicity research are still based on traditional static two- or three-dimensional cell culture, although these means could investigate some toxic chemicals induced hepatotoxicity, but most of these toxicities failed to reappear in human, at least not in similar or calculable dose level. These failures may cause by the monoculture of only hepatocytes, ignored the signal communication to other non-parenchymal cells in liver tissue, also other complex microenvironment such as endothelial barrier, shear stress and other factors which were really existed in vivo but absent here, final leading to a low reliability of experimental results. In this study, a three-dimensional dynamic multi-cellular liver-on-a-chip device (3D-DMLoC) was developed to reproduce the microenvironment of in vivo liver tissue, including the simulation of hepatic sinusoid, perisinusoidal space and continuous liquid perfusion, hepatocytes could gather to some 3D cell spheroids in this chip. The perfusion could bring a real-time exchange of chemicals, nutrients, metabolites, supply suitable oxygen and a weak shear stress. The pressure and oxygen distribution inner the chip were simulated and evaluated by COMSOL Multiphysics software. HepaRG were co-cultured with HUVEC for 7 days in this chip, expression of hepatic polarization protein ZO-1 and MRP2, liver function factors ALB, UREA and CYP450s were almost all higher than in traditional static culture. Several drugs and heavy metal ions induced hepatotoxicity were then investigated, LDH released from hepatocyte spheroids in mostly 3D-DMLoC groups were higher than same-dosed 2D group, indicated the spheroids were more sensibility to the toxins. The hepatoxicity might be induced by acute hepatocytes injury according to the ratios of secreted AST/ALT contents. In conclusion, a liver-on-a-chip device was successfully developed and verified for better reproducing the in vivo physiological microenvironment of liver. It could be applied for easily, efficiently, and accurately screening the potential hepatotoxic chemicals in future.

    Towards potentiometric detection in nonaqueous media: Evaluation of the impacts of organic solvents on polymeric membrane ion-selective electrodes

    Lin Z.Liang R.Qin W.
    5页
    查看更多>>摘要:? 2022 Elsevier B.V.Polymeric membrane ion-selective electrodes (ISEs) have been widely used in various fields including clinical diagnosis, environmental monitoring and industrial analysis. Although most samples of analytical interest measured by the ISEs are aqueous solutions, the applications of these electrodes in nonaqueous media are often inevitable. Unfortunately, so far, little has been known about the extent to which the properties of the ISEs could be affected by the organic solvents. Herein, the feasibility for the applications of the polymeric membrane ISEs in nonaqueous media has been investigated. A polymeric membrane Ca2+-ISE is chosen as a model of potentiometric sensors. Four typical water miscible organic solvents (three protic solvents: ethanol, acetic acid, and methanol, and one aprotic dipolar solvent: acetonitrile) are used as the representative examples. Experiments show that the aprotic solvent acetonitrile has the strongest destructive ability towards the sensing performance of the ISE in terms of Nernstian slope and selectivity coefficient. Moreover, the effect on the sensing performance depends on the kind of the protic solvent, the immersion time and the polarity of the membrane plasticizer. We believe that the obtained results could promote further applications of the polymeric membrane ISEs in the organic solvent-containing samples, which could significantly extend the application scope of the ISEs.