Showing papers in "Analytical Chemistry in 2017"
TL;DR: This paper presents a meta-analysis of the ECL Nanomaterial System and its applications and discusses the methods used to develop and evaluate these systems and the techniques used to fabricate these systems.
Abstract: ■ CONTENTS Novel ECL Systems 358 Novel Organic Luminophores 358 Novel Inorganic Luminophores 359 Novel Nanomaterial System 360 Detection Methodologies and Signaling Amplification Strategies 361 General Detection Methodologies 361 Novel Signal Amplification Strategies 361 ECL Applications 362 Metal Ions Detection 362 Small Molecules Detection 362 ECL Immunoassay 363 ECL Genosensors 365 ECL Cytosensors 366 Conclusions and Outlooks 368 Author Information 369 Corresponding Author 369 ORCID 369 Author Contributions 369 Notes 369 Biographies 369 Acknowledgments 369 References 369
405 citations
TL;DR: This work focuses on three-Dimensional Electrochemical Detection, which automates the very labor-intensive and therefore time-heavy and expensive process of characterize and characterize the electrochemical activity of the response of the immune system.
Abstract: Applications Yuanyuan Yang,† Eka Noviana,† Michael P. Nguyen,† Brian J. Geiss,‡ David S. Dandy, and Charles S. Henry*,†,§ †Department of Chemistry, Colorado State University, Fort Collins, Colorado 80523, United States ‡Department of Microbiology, Immunology, and Pathology, Colorado State University, Fort Collins, Colorado 80523, United States Department of Chemical and Biological Engineering, Colorado State University, Fort Collins, Colorado 80523, United States ■ CONTENTS Fabrication 71 Hydrophobic/Solvent Barrier 72 Deposition 73 Flow and Injection Control 74 Three-Dimensional Devices 75 Incorporating Nonsensing Electrodes 75 Colorimetric Detection 75 Detectors and Readout 75 Reflectance-Based Measurement 75 Transmittance-Based Measurement 77 Instrument-Free Measurement 77 Biomedical Applications 77 Enzymatic Methods 77 Immunoassays 78 Other 79 Environmental Applications 79 Other Applications 80 Electrochemical Detection 80 Electrodes 80 Carbon Electrodes 81 Metallic Electrodes 81 Biological Applications 82 Glucose Sensors 82 Immunosensors 84 Other Examples 84 Environmental Applications 84 Other Technologies 85 Chemiluminescence and Electrochemiluminescence 85 Fluorescence 85 Surface-Enhanced Raman Spectroscopy 85 Separation 86 Preconcentration 86 Conclusions and Future Directions 87 Author Information 87 Corresponding Author 87 ORCID 87 Notes 87 Biographies 87 Acknowledgments 88 References 88
388 citations
TL;DR: This paper presents a meta-modelling framework for estimating the modeled response of the immune system to various types of injury and shows clear patterns of decline in response to certain types of injuries.
Abstract: Samiksha Nayak,†,§ Nicole R. Blumenfeld,†,§ Tassaneewan Laksanasopin,‡ and Samuel K. Sia*,† †Department of Biomedical Engineering, Columbia University, 351 Engineering Terrace, 1210 Amsterdam Avenue, New York, New York 10027, United States ‡Biological Engineering Program, Faculty of Engineering, King Mongkut’s University of Technology Thonburi, 126 Pracha Uthit Road, Bang Mod, Thung Khru, Bangkok 10140, Thailand
369 citations
TL;DR: An all-in-one paper-based analytical device was successfully developed for visual fluorescence detection of carcinoembryonic antigen (CEA) on CdTe/CdSe quantum dot (QD)-enzyme-impregnated paper by coupling with a bioresponsive controlled-release system from DNA-gated mesoporous silica nanocontainers (MSNs).
Abstract: An all-in-one paper-based analytical device (PAD) was successfully developed for visual fluorescence detection of carcinoembryonic antigen (CEA) on CdTe/CdSe quantum dot (QD)-enzyme-impregnated paper by coupling with a bioresponsive controlled-release system from DNA-gated mesoporous silica nanocontainers (MSNs). The assay was carried out in a centrifuge tube by using glucose-loaded MSNs with a CEA aptamer and a QD-enzyme-paper attached on the lid. Initially, single-strand complementary DNA to a CEA aptamer was covalently conjugated to the aminated MSN, and then glucose (enzyme substrate) molecules were gated into the pore with the help of the aptamer. Glucose oxidase (GOD) and CdTe/CdSe QDs were coimmobilized on paper for the visual fluorescence signal output. Upon target CEA introduction in the detection cell, the analyte specifically reacted with the immobilized aptamer on the MSN to open the pore, thereby resulting in the glucose release. The released glucose was oxidized by the immobilized GOD on pap...
350 citations
TL;DR: The developed immunoassay exhibited good reproducibility and acceptable accuracy, and the method accuracy relative to AFB1 ELISA kit was evaluated for analyzing naturally contaminated or spiked peanut samples, giving the well-matched results between two methods.
Abstract: Aflatoxin B1 (AFB1) monitoring has attracted extensive attention because food safety is a worldwide public health problem. Herein, we design a novel simultaneously visual and photoelectrochemical (PEC) immunosensing system for rapid sensitive detection of AFB1 in foodstuff. The immunoreaction was carried out on anti-AFB1 antibody-modified magnetic beads by using glucose oxidase (GOx)-labeled AFB1-bovine serum albumin (AFB1–BSA) conjugates as the tags with a competitive-type immunoassay format, while the visual and PEC evaluation was performed via carbon quantum dots (CQDs)-functionalized MnO2 nanosheets. Accompanying the formation of immunocomplexes, the carried GOx initially oxidized the substrate (glucose) for the generation of H2O2, which reduced/etched MnO2 nanosheets into Mn2+ ions, thereby resulting in the dissociation of CQDs from the electrode. Within the applied potentials, the photocurrent of MnO2-CQDs-modified electrode decreased with the increasing H2O2 level in the detection cell. Meanwhile, ...
329 citations
TL;DR: Improvements on the measurement accuracy of experimental parameters influencing IM separations provide standardized drift tube, nitrogen CCS values (DTCCSN2) for over 120 unique ion species with the lowest measurement uncertainty to date.
Abstract: Collision cross section (CCS) measurements resulting from ion mobility–mass spectrometry (IM-MS) experiments provide a promising orthogonal dimension of structural information in MS-based analytical separations. As with any molecular identifier, interlaboratory standardization must precede broad range integration into analytical workflows. In this study, we present a reference drift tube ion mobility mass spectrometer (DTIM-MS) where improvements on the measurement accuracy of experimental parameters influencing IM separations provide standardized drift tube, nitrogen CCS values (DTCCSN2) for over 120 unique ion species with the lowest measurement uncertainty to date. The reproducibility of these DTCCSN2 values are evaluated across three additional laboratories on a commercially available DTIM-MS instrument. The traditional stepped field CCS method performs with a relative standard deviation (RSD) of 0.29% for all ion species across the three additional laboratories. The calibrated single field CCS method...
315 citations
309 citations
TL;DR: A direct experimental comparison of the three 3D printing technologies dominating microfluidics was conducted using a Y-junction micro fluidic device, the design of which was optimized for each printer: fused deposition molding (FDM), Polyjet, and digital light processing stereolithography (DLP-SLA).
Abstract: Three-dimensional (3D) printing has emerged as a potential revolutionary technology for the fabrication of microfluidic devices. A direct experimental comparison of the three 3D printing technologies dominating microfluidics was conducted using a Y-junction microfluidic device, the design of which was optimized for each printer: fused deposition molding (FDM), Polyjet, and digital light processing stereolithography (DLP-SLA). Printer performance was evaluated in terms of feature size, accuracy, and suitability for mass manufacturing; laminar flow was studied to assess their suitability for microfluidics. FDM was suitable for microfabrication with minimum features of 321 ± 5 μm, and rough surfaces of 10.97 μm. Microfluidic devices >500 μm, rapid mixing (71% ± 12% after 5 mm, 100 μL/min) was observed, indicating a strength in fabricating micromixers. Polyjet fabricated channels with a minimum size of 205 ± 13 μm, and a surface roughness of 0.99 μm. Compared with FDM, mixing decreased (27% ± 10%), but Polyjet printing is more suited for microfluidic applications where flow splitting is not required, such as cell culture or droplet generators. DLP-SLA fabricated a minimum channel size of 154 ± 10 μm, and 94 ± 7 μm for positive structures such as soft lithography templates, with a roughness of 0.35 μm. These results, in addition to low mixing (8% ± 1%), showed suitability for microfabrication, and microfluidic applications requiring precise control of flow. Through further discussion of the capabilities (and limitations) of these printers, we intend to provide guidance toward the selection of the 3D printing technology most suitable for specific microfluidic applications.
276 citations
TL;DR: A paper-based colorimetric assay for DNA detection based on pyrrolidinyl peptide nucleic acid (acpcPNA)-induced nanoparticle aggregation is reported as an alternative to traditional colorimetry approaches.
Abstract: The development of simple fluorescent and colorimetric assays that enable point-of-care DNA and RNA detection has been a topic of significant research because of the utility of such assays in resource limited settings. The most common motifs utilize hybridization to a complementary detection strand coupled with a sensitive reporter molecule. Here, a paper-based colorimetric assay for DNA detection based on pyrrolidinyl peptide nucleic acid (acpcPNA)-induced nanoparticle aggregation is reported as an alternative to traditional colorimetric approaches. PNA probes are an attractive alternative to DNA and RNA probes because they are chemically and biologically stable, easily synthesized, and hybridize efficiently with the complementary DNA strands. The acpcPNA probe contains a single positive charge from the lysine at C-terminus and causes aggregation of citrate anion-stabilized silver nanoparticles (AgNPs) in the absence of complementary DNA. In the presence of target DNA, formation of the anionic DNA-acpcPN...
274 citations
TL;DR: This paper presents a meta-analysis of 3D printing techniques and applications using a comparison of the techniques used in fused deposition modeling and selective laser sintering to evaluate the properties of these techniques and their applications.
Abstract: ■ CONTENTS Traditional Fabrication Techniques 57 Benefits of 3D Printing 58 3D Printing Techniques and Applications 59 Stereolithography 59 Technology 59 Applications 59 Selective Laser Sintering 61 Technology 61 Applications 61 Inkjet and Polyjet Printing 62 Technology 62 Applications 62 Fused Deposition Modeling 64 Technology 64 Applications 64 Laminated Object Manufacturing 65 Technology 65 Applications 65 Direct Printing 65 Metal Printers 65 Wire-Feed Additive Manufacturing 65 Applications 65 Bioprinters 66 Technology 66 Applications 67 Automation 67 Selecting a Printer 67 Conclusions and Future Directions 67 Author Information 68 Corresponding Author 68 ORCID 68 Author Contributions 68 Notes 68 Biographies 68 References 68
247 citations
TL;DR: A selective fluorescent nanoprobe for Fe3+ detection in biological samples based on ultrabright N/P codoped carbon dots that showed high fluorescence, good accuracy, and excellent selectivity, which presents the potential practical application for diagnosis ofFe3+ related disease.
Abstract: Measuring the levels of Fe3+ in human body has attracted considerable attention for health monitoring as it plays an essential role in many physiological processes. In this work, we reported a selective fluorescent nanoprobe for Fe3+ detection in biological samples based on ultrabright N/P codoped carbon dots. By employing adenosine 5′-triphosphate (ATP) as the carbon, nitrogen, and phosphorus source, the N/P codoped carbon dots could be simply prepared through hydrothermal treatment. The obtained carbon dots exhibited high quantum yields up to 43.2%, as well as excellent photostability, low toxicity, and water solubility. Because of the Fe–O–P bonds formed between Fe3+ and the N/P codoped carbon dots, this nanoprobe showed high selectivity toward Fe3+ against various potential interfering substances in the presence of EDTA. The fluorescence quenching of as-fabricated carbon dots was observed with the increasing Fe3+ concentration, and the calibration curve displayed a wide linear region over the range of...
TL;DR: New algorithms that carry out the sequential construction of EICs and detection of E IC peaks are developed and evidence that these new algorithms detect significantly fewer false positives is presented.
Abstract: False positive and false negative peaks detected from extracted ion chromatograms (EIC) are an urgent problem with existing software packages that preprocess untargeted liquid or gas chromatography–mass spectrometry metabolomics data because they can translate downstream into spurious or missing compound identifications. We have developed new algorithms that carry out the sequential construction of EICs and detection of EIC peaks. We compare the new algorithms to two popular software packages XCMS and MZmine 2 and present evidence that these new algorithms detect significantly fewer false positives. Regarding the detection of compounds known to be present in the data, the new algorithms perform at least as well as XCMS and MZmine 2. Furthermore, we present evidence that mass tolerance in m/z should be favored rather than mass tolerance in ppm in the process of constructing EICs. The mass tolerance parameter plays a critical role in the EIC construction process and can have immense impact on the detection ...
TL;DR: An upper bound on the number of unique metabolites detected in Escherichia coli samples analyzed with one untargeted metabolomics method is placed and the creDBle database is introduced, which contains accurate mass, retention time, and MS/MS fragmentation data as well as annotations of all credentialed features.
Abstract: When using liquid chromatography/mass spectrometry (LC/MS) to perform untargeted metabolomics, it is now routine to detect tens of thousands of features from biological samples. Poor understanding of the data, however, has complicated interpretation and masked the number of unique metabolites actually being measured in an experiment. Here we place an upper bound on the number of unique metabolites detected in Escherichia coli samples analyzed with one untargeted metabolomics method. We first group multiple features arising from the same analyte, which we call “degenerate features”, using a context-driven annotation approach. Surprisingly, this analysis revealed thousands of previously unreported degeneracies that reduced the number of unique analytes to ∼2961. We then applied an orthogonal approach to remove nonbiological features from the data using the 13C-based credentialing technology. This further reduced the number of unique analytes to less than 1000. Our 90% reduction in data is 5-fold greater tha...
TL;DR: This tutorial discusses the motivations for doing two-dimensional liquid chromatography and describes the commonly used implementations of the method, and discusses the state of the art in 2D-LC performance as measured by peak capacity.
Abstract: In this tutorial, we discuss the motivations for doing two-dimensional liquid chromatography (2D-LC) and describe the commonly used implementations of the method. We review important guiding principles for method development, discuss the state of the art in 2D-LC performance as measured by peak capacity, and describe example applications from different fields that we hope will inspire new users to adopt 2D-LC for their analytical problems.
TL;DR: Because of the low cytotoxicity, good optical and colloidal stability, and excellent wavelength dependent sensitivity and selectivity toward lysine and pH, this probe was successfully applied to monitor the dynamic variation of lysines and pH in cellular systems, demonstrating the promising applicability for biosensing in the future.
Abstract: Recently, the development of new fluorescent probes for the ratiometric detection of target objects inside living cells has received great attention. Normally, the preparation, modification as well as conjugation procedures of these probes are complicated. On this basis, great efforts have been paid to establish convenient method for the preparation of dual emissive nanosensor. In this work, a functional dual emissive carbon dots (dCDs) was prepared by a one-pot hydrothermal carbonization method. The dCDs exhibits two distinctive fluorescence emission peaks at 440 and 624 nm with the excitation at 380 nm. Different from the commonly reported dCDs, this probe exhibited an interesting wavelength dependent dual responsive functionality toward lysine (440 nm) and pH (624 nm), enabling the ratiometric detection of these two targets. The quantitative analysis displayed that a linear range of 0.5-260 μM with a detection limit of 94 nM toward lysine and the differentiation of pH variation from 1.5 to 5.0 could be readily realized in a ratiometric strategy, which was not reported before with other carbon dots (CDs) as the probe. Furthermore, because of the low cytotoxicity, good optical and colloidal stability, and excellent wavelength dependent sensitivity and selectivity toward lysine and pH, this probe was successfully applied to monitor the dynamic variation of lysine and pH in cellular systems, demonstrating the promising applicability for biosensing in the future.
TL;DR: It is reported that boric acid is used to tune the optical properties of lanthanide metal-organic frameworks (LMOFs) for dual-fluorescence emission and improves the selectivity of L MOFs for the determination of F- ions and rational selection of functional ligands can improve the sensing efficiency of LMOFs through tuning their optical property and enhancing the selectivities toward targets.
Abstract: Here, we report that boric acid is used to tune the optical properties of lanthanide metal–organic frameworks (LMOFs) for dual-fluorescence emission and improves the selectivity of LMOFs for the determination of F– ions. The LMOFs are prepared with 5-boronoisophthalic acid (5-bop) and Eu3+ ions as the precursors. Emission mechanism study indicates that 5-bop is excited with UV photons to produce its triplet state, which then excites Eu3+ ions for their red emission. This is the general story of the antenna effect, but electron-deficient boric acid decreases the energy transfer efficiency from the triplet state of 5-bop to Eu3+ ions, so dual emission from both 5-bop and Eu3+ ions is efficiently excited at the single excitation of 275 nm. Moreover, boric acid is used to identify fluoride specifically as a free accessible site. The ratiometric fluorescent detection of F– ions is validated with the dual emission at single excitation. The LMOFs are very monodisperse, so the determination of aqueous F– ions is ...
TL;DR: An automated computational framework to annotate ions for possible chemical identity using a multistage clustering algorithm in which metabolic pathway associations are used along with intensity profiles, retention time characteristics, mass defect, and isotope/adduct patterns is described.
Abstract: Improved analytical technologies and data extraction algorithms enable detection of >10 000 reproducible signals by liquid chromatography–high-resolution mass spectrometry, creating a bottleneck in chemical identification. In principle, measurement of more than one million chemicals would be possible if algorithms were available to facilitate utilization of the raw mass spectrometry data, especially low-abundance metabolites. Here we describe an automated computational framework to annotate ions for possible chemical identity using a multistage clustering algorithm in which metabolic pathway associations are used along with intensity profiles, retention time characteristics, mass defect, and isotope/adduct patterns. The algorithm uses high-resolution mass spectrometry data for a series of samples with common properties and publicly available chemical, metabolic, and environmental databases to assign confidence levels to annotation results. Evaluation results show that the algorithm achieves an F1-measure ...
TL;DR: A straightforward and convenient fluorescent filter paper sensor was developed for the detection of TNP, providing a valuable platform for TNP sensing in public safety and security.
Abstract: Because 2,4,6-trinitrophenol (TNP) and its analogues such as 2,4,6-trinitrotoluene (TNT) possess similar chemical structures and properties, the reliable and accurate detection of TNP from its analogues still remains a challenging task. In the present work, a selective and sensitive method based on the water-soluble silicon nanoparticles (SiNPs) for the determination of TNP was established. The SiNPs with good thermostability and excellent antiphotobleaching capability were prepared via a simple one-pot method. Compared with the synthesized time of other nanomaterials with respect to the detection of TNP, this method avoided a multistep and time-consuming synthesis procedure. Significantly, the fluorescence of the SiNPs could be remarkably quenched by TNP via an inner filter effect. A wide linear range was obtained from 0.02 to 120 μg/mL with a limit of detection of 6.7 ng/mL. The method displayed excellent selectivity toward TNP over other nitroaromatic explosives. The proposed fluorescent method was suc...
TL;DR: A dual mode fluorescent probe, which is based on an integration of fluorescein and coumarin fluorophores, was developed for the discrimination of Cys from Hcy and GSH and shows the advantage of quick reaction with Cys, resulting in a strong fluorescence turn-on response when excited at 450 nm.
Abstract: A dual mode fluorescent probe, which is based on an integration of fluorescein and coumarin fluorophores, was developed for the discrimination of Cys from Hcy and GSH. This probe (2) shows the advantage of quick reaction (5 min) with Cys, resulting in a strong fluorescence turn-on response when excited at 450 nm. Notably, it also demonstrates the ratiometric fluorescence property while excited by a shorter wavelength (332 nm). All of results suggest probe 2 has a high selectivity toward Cys even in the presence of other amino acids, cations and anions. The detection limit of Cys was calculated as 0.084 μM, which was much lower than the intracellular concentration. 1H NMR, MS and DFT calculation were used to reveal the detection mechanism further. Finally, this low cytotoxic probe was successfully applied in bioimaging within HepG2 cells.
TL;DR: The first dual-detection fluorescent probe Mito-VH is designed and sythesized that can visualize viscosity and H2O2 in mitochondria with different fluorescence signals in living cells and prevents the twisted internal charge transfer (TICT) process.
Abstract: Mitochondria, as essential and interesting organelles within the eukaryotic cells, play key roles in a variety of pathologies, and its abnormalities are closely associated with Alzheimer’s disease (AD) and other diseases. Studies have shown that the abnormal of viscosity and concentration of hydrogen peroxide in mitochondria were all associated with AD. Accordingly, the detection of viscosity and hydrogen peroxide in mitochondria has attracted great attention. However, it remains a great challenge to explore a single probe, which can dual-detect the viscosity and H2O2 in mitochondria. Herein, in two ways to prevent the twisted internal charge transfer (TICT) process, we designed and sythesized the first dual-detection fluorescent probe Mito-VH that can visualize viscosity and H2O2 in mitochondria with different fluorescence signals in living cells.
TL;DR: This is the first report of simultaneous detection of two different DNA mixtures using a SERS-based LFA platform, and this novel detection technique is also a promising multiplex DNA sensing platform for early disease diagnosis.
Abstract: A new class of surface-enhanced Raman scattering (SERS)-based lateral flow assay (LFA) biosensor has been developed for the simultaneous detection of dual DNA markers. The LFA strip in this sensor was composed of two test lines and one control line. SERS nano tags labeled with detection DNA probes were used for quantitative evaluation of dual DNA markers with high sensitivity. Target DNA, associated with Kaposi’s sarcoma-associated herpesvirus (KSHV) and bacillary angiomatosis (BA), were tested to validate the detection capability of this SERS-based LFA strip. Characteristic peak intensities of SERS nano tags on two test lines were used for quantitative evaluations of KSHV and BA. The limits of detection for KSHV and BA, determined from our SERS-based LFA sensing platform, were estimated to be 0.043 and 0.074 pM, respectively. These values indicate approximately 10 000 times higher sensitivity than previously reported values using the aggregation-based colorimetric method. We believe that this is the firs...
TL;DR: It is found that ssDNA adsorbed on g-C3N4 NSs could improve the catalytic activity of the nanosheets and demonstrates the high potential of the ssDNA-NSs hybrid in clinical diagnosis using liquid biopsy.
Abstract: The present work investigates the capability of single-stranded DNA (ssDNA) in enhancing the intrinsic peroxidase-like activity of the g-C3N4 nanosheets (NSs). We found that ssDNA adsorbed on g-C3N4 NSs could improve the catalytic activity of the nanosheets. The maximum reaction rate of the H2O2-mediated TMB oxidation catalyzed by the ssDNA-NSs hybrid was at least 4 times faster than that obtained with unmodified NSs. The activity enhancement could be attributed to the strong interaction between TMB and ssDNA mediated by electrostatic attraction and aromatic stacking and by both the length and base composition of the ssDNA. The high catalytic activity of the ssDNA-NSs hybrid permitted sensitive colorimetric detection of exosomes if the aptamer against CD63, a surface marker of exosome, was employed in hybrid construction. The sensor recognized the differential expression of CD63 between the exosomes produced by a breast cancer cell line (MCF-7) and a control cell line (MCF-10A). Moreover, a similar trend was detected in the circulating exosomes isolated from the sera samples collected from breast cancer patients and healthy controls. Our work sheds lights on the possibility of using ssDNA to enhance the peroxidase-like activity of nanomaterials and demonstrates the high potential of the ssDNA-NSs hybrid in clinical diagnosis using liquid biopsy.
TL;DR: By taking advantages of biocompatibility and diagnostic property enabled by AG73-MOF nanosheets, the elimination process of Hep in live rats is quantitatively monitored by coupling with microdialysis technology.
Abstract: Metal–organic framework (MOF) nanosheets are a class of two-dimensional (2D) porous and crystalline materials that hold promise for catalysis and biodetection. Although 2D MOF nanosheets have been utilized for in vitro assays, ways of engineering them into diagnostic tools for live animals are much less explored. In this work, a series of MOF nanosheets are successfully engineered into a highly sensitive and selective diagnostic platform for in vivo monitoring of heparin (Hep) activity. The iron-porphyrin derivative is selected as a ligand to synthesize a series of archetypical MOF nanosheets with intrinsic heme-like catalytic sites, mimicking peroxidase. Hep-specific AG73 peptides as recognition motifs are physically adsorbed onto MOF nanosheets, blocking active sites from nonspecific substrate–catalyst interaction. Because of the highly specific interaction between Hep and AG73, the activity of AG73-MOF nanosheets is restored upon the binding of Hep, but not Hep analogues and other endogenous biomolecul...
TL;DR: A gecko-inspired nanotentacle surface-enhanced Raman spectroscopy (G-SERS) platform is proposed for the first time for the simultaneous detection of three kinds of pesticides via a simple and intuitive "press and peeled-off" approach.
Abstract: Rapid sampling and multicomponent detection are crucial for monitoring of pesticide residues analysis. Here, a gecko-inspired nanotentacle surface-enhanced Raman spectroscopy (G-SERS) platform is proposed for the first time for the simultaneous detection of three kinds of pesticides via a simple and intuitive “press and peeled-off” approach. The G-SERS platform obtained from seeding deposition of silver nanoparticles (Ag NPs) on 3D PDMS nanotentacle array is flexible and free-standing. Compared with other substrates, this G-SERS substrate can simultaneously provide outstanding SERS activity (enhancement factor = 1.2 × 107), superior reproducibility (RSD = 5.8%) and countless flexible nanoscale “tentacles” (∼6.7 × 108/cm2). Moreover, the high density of “tentacles” can freely approach the microarea and enable efficient target collection, which were confirmed by SEM and HPLC. By direct sampling from cucumber, apple, and grape surfaces, thiram (TMTD), methyl parathion (MPT), malachite green (MG), and their m...
TL;DR: A DNA-mediated gold-silver nanomushroom with interior nanogaps directly synthesized and used for multiplex and simultaneous SERS detection of various DNA and RNA targets is reported.
Abstract: Uniform silver-containing metal nanostructures with strong and stable surface-enhanced Raman scattering (SERS) signals hold great promise for developing ultrasensitive probes for biodetection. Nevertheless, the direct synthesis of such ready-to-use nanoprobes remains extremely challenging. Herein we report a DNA-mediated gold–silver nanomushroom with interior nanogaps directly synthesized and used for multiplex and simultaneous SERS detection of various DNA and RNA targets. The DNA involved in the nanostructures can act as not only gap DNA (mediated DNA) but also probe DNA (hybridized DNA), and DNA’s involvement enables the nanostructures to have the inherent ability to recognize DNA and RNA targets. Importantly, we were the first to establish a new method for the generation of multicolor SERS probes using two different strategies. First Raman-labeled alkanethiol probe DNA was assembled on gold nanoparticles, and second, thiol-containing Raman reporters were coassembled with the probe DNA. The ready-to-us...
TL;DR: A two-photon reversible fluorescent probe L1 was designed and synthesized and successfully applied to detect intracellular HClO in lysosome, showing great selectivity for hypochlorous acid over other reactive oxygen species (ROS) and anions.
Abstract: A two-photon reversible fluorescent probe L1 was designed and synthesized. The fluorescence intensity of the probe solution was strong, while the fluorescence of the solution was obviously quenched and the color of the solution was changed after the addition of hypochlorous acid, indicating this is “naked-eye sensor” for the detection of HClO. The probe showed great selectivity for hypochlorous acid over other reactive oxygen species (ROS) and anions. Fluorescence titration experiments showed that the probe has a low detection limit of 0.674 μM. Because of a morpholine group introduced to the naphathalimide framework, probe L1 was successfully applied to detect intracellular HClO in lysosome.
TL;DR: This is the first interlaboratory assessment of a widely used, targeted metabolomics assay illustrating the reproducibility of the protocol and how data generated on different instruments could be directly integrated in large-scale epidemiological studies.
Abstract: A critical question facing the field of metabolomics is whether data obtained from different centers can be effectively compared and combined. An important aspect of this is the interlaboratory precision (reproducibility) of the analytical protocols used. We analyzed human samples in six laboratories using different instrumentation but a common protocol (the AbsoluteIDQ p180 kit) for the measurement of 189 metabolites via liquid chromatography (LC) or flow injection analysis (FIA) coupled to tandem mass spectrometry (MS/MS). In spiked quality control (QC) samples 82% of metabolite measurements had an interlaboratory precision of <20%, while 83% of averaged individual laboratory measurements were accurate to within 20%. For 20 typical biological samples (serum and plasma from healthy individuals) the median interlaboratory coefficient of variation (CV) was 7.6%, with 85% of metabolites exhibiting a median interlaboratory CV of <20%. Precision was largely independent of the type of sample (serum or plasma) ...
TL;DR: Improved in instrument parameters and natural isotope correction enable more accurate measurement of metabolite labeling and thus metabolic flux, and presents an algorithm and associated open-source code, named AccuCor, for this purpose.
Abstract: Orbitraps are high-resolution ion-trap mass spectrometers that are widely used in metabolomics. While the mass accuracy and resolving power of orbitraps have been extensively documented, their spectral accuracy, i.e., accuracy in measuring the abundances of isotopic peaks, remains less studied. In analyzing spectra of unlabeled metabolites, we discovered a systematic under representation of heavier natural isotopic species, especially for high molecular weight metabolites (∼20% under-measurement of [M + 1]/[M + 0] ratio at m/z 600). We hypothesize that these discrepancies arise for metabolites far from the lower limit of the mass scan range, due to the weaker containment in the C-trap that results in suboptimal trajectories inside the Orbitrap analyzer. Consistent with this, spectral fidelity was restored by dividing the mass scan range (initially 75 m/z to 1000 m/z) into two scan events, one for lower molecular weight and the other for higher molecular weight metabolites. Having thus obtained accurate ma...