34,738 results match your criteria Analytical chemistry[Journal]


A ratio-based method to identify true biomarkers by normalizing circulating ncRNA sequencing and quantitative PCR data.

Anal Chem 2019 Apr 19. Epub 2019 Apr 19.

Recent studies have indicated that circulating noncoding RNAs (ncRNAs) such as miRNAs are stable biomarkers for the diagnosis and prognosis of human diseases. However, due to low concentration of circulating ncRNAs in blood, data normalization in plasma/serum ncRNA experiments using next-generation sequencing and quantitative real time RT-qPCR is a challenge. We found that the current normalization methods based on synthetic external spiked-in controls or published endogenous miRNA controls are inappropriate as they are not stably expressed and therefore, fails to reliably detect differentially expressed ncRNAs. Read More

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http://pubs.acs.org/doi/10.1021/acs.analchem.9b00821
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http://dx.doi.org/10.1021/acs.analchem.9b00821DOI Listing
April 2019
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Sulfur Regulated BN QDs Electrochemiluminescence with Amplified Surface Plasmon Coupling Strategy for BRAF gene Detection.

Anal Chem 2019 Apr 19. Epub 2019 Apr 19.

Because BN QD has a wide-gap (5.0-6.0 eV) than other QDs, the edge configurations, chemical functionalities and heteroatom dopants can decrease and regulated the band gap of BN QDs thereby ameliorating the QDs properties. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00965DOI Listing

Boronic Derivatization of Monoacylglycerol and Monitoring in Biofluids.

Anal Chem 2019 Apr 19. Epub 2019 Apr 19.

Monoacylglycerols (MAGs) are active mediators involved in multiple biological processes closely related to the pathological de-velopment of diabetes, obesity and cancers. Sensitive and unambiguous detection of MAG is thus essential; however, previous methods are both indirect and labor-intensive. Herein, we developed a straightforward approach by derivatization of MAGs with 3-nitrophenylboronic acid (3-NPB) for sensitive and selective analysis in cell lysates, tissues and serums by mass spectrometry (MS). Read More

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http://pubs.acs.org/doi/10.1021/acs.analchem.9b00805
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http://dx.doi.org/10.1021/acs.analchem.9b00805DOI Listing
April 2019
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Ratiometric Fluorescent Quantification of the Size-Dependent Cellular Toxicity of Silica Nanoparticles.

Anal Chem 2019 Apr 19. Epub 2019 Apr 19.

Nanoscale particles are ubiquitous in the atmosphere, and the widespread use of nanoparticles may increase the risks of organ damage. Therefore, it is of great significance to investigate the toxicity of nanoparticles of different sizes toward living cells, especially lung epithelial cells. In this study, the quantitative ratiometric fluorescent detection of intracellular pH changes was utilized to evaluate the cytotoxicity of mesoporous silica nanoparticles of different sizes after the nanoparticles had entered lung epithelial cells. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00633DOI Listing

Conformationally Induced Off-On Two-photon Fluorescent Bioprobes for Dynamically Tracking the Interactions among Multiple Organelles.

Anal Chem 2019 Apr 19. Epub 2019 Apr 19.

Unveiling the synergism among multiple organelles for fully exploring the mysteries of the cell has drawn more and more attention. Herein, we developed two two-photon fluorescent bioprobes (Lyso-TA and Mito-QA), of which the conformational change triggered "off-on" fluorescent response. Lyso-TA can real-time monitor the fusion and movement of lysosomes, as well as unveil the mitophagy process with the engagement of lysosomes. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00806DOI Listing

A Facile, Versatile, and Highly Efficient Strategy for Peroxynitrite Bioimaging Enabled by Formamide Deformylation.

Anal Chem 2019 Apr 19. Epub 2019 Apr 19.

Peroxynitrite (ONOO-) is attracting increasing attention due to its involvement in multiple facets of pathophysiological processes. However, ONOO- bioimaging are still challenging due to (1) the lack of highly specific reaction triggers, (2) the tedious and low-yielding synthesis of current sophisticated probes, and (3) the lack of availability of a versatile chemical strategy. To address these challenges, based on the amine formylation/deformylation chemistry, we have developed a novel strategy for ONOO- bioimaging. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b01175DOI Listing

Image-based quantification of cell debris as a measure of apoptosis.

Anal Chem 2019 Apr 19. Epub 2019 Apr 19.

Apoptosis is a controlled form of cell death that can be induced by various diseases and exogenous toxicants. Common apoptosis detection methods rely on fluorescent markers, which necessitates the use of costly reagents and time-consuming labeling procedures. Label-free methods avoid these problems, but often require specialized instruments instead. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b01243DOI Listing

Direct Mass Spectrometry Analysis Using In-Capillary Dicationic Ionic Liquid-Based in situ Dispersive Liquid-Liquid Microextraction and Sonic-Spray Ionization.

Anal Chem 2019 Apr 19. Epub 2019 Apr 19.

The current study reports on a direct mass spectrometry (MS) analysis method using in-capillary dicationic ionic liquid (DIL)-based in situ dispersive liquid-liquid microextraction (DLLME) and sonic-spray ionization (SSI). The developed method merged extraction, enrichment, ionization, and detection of perfluorinated compounds (PFCs) in environmental water into a single step. A microliter-scale ternary fluidic system was designed and integrated into a disposable pulled capillary, in which an imidazolium-based germinal DIL reagent activated an in situ metathesis reaction. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00597DOI Listing

Synthetic Small Molecule Characterization and Isomer Discrimination Using Gas-phase Hydrogen-Deuterium Exchange IMS-MS.

Anal Chem 2019 Apr 19. Epub 2019 Apr 19.

Ion mobility spectrometry-mass spectrometry (IMS-MS) combined with gas-phase hydrogen deuterium exchange has been used to characterize novel psychoactive substances (NPSs) which are small synthetic compounds designed to mimic the effects of other illicit substances. Here, NPSs containing labile heteroatom hydrogens were evaluated for HDX reactivity in the presence of either deuterated water (D2O) or ammonia (ND3) within the drift tube. An initial evaluation of exchange propensity was performed for six NPSs. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00979DOI Listing

Rapid fragmentation during seeded lysozyme aggregation revealed at the single molecule level.

Anal Chem 2019 Apr 19. Epub 2019 Apr 19.

Protein aggregation is associated with neurodegenerative disorders such as Alzheimer's and Parkinson's diseases. The poorly understood pathogenic mechanism of amyloid diseases makes early-stage diagnostics or therapeutic intervention a challenge. Seeded polymerisation that reduces the duration of the lag phase and accelerates fibril growth is a widespread model to study amyloid formation. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b01221DOI Listing
April 2019
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Boric Acid-Functionalized Covalent-Organic Framework for Specific Enrichment and Direct Detection of Cis-Diol-Containing Compounds by Matrix-Assisted Laser Desorption/Ionization Time-of-Flight Mass Spectrometry.

Anal Chem 2019 Apr 19. Epub 2019 Apr 19.

Design and synthesis of novel matrix while serving as high selective adsorption materials are significant for the matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS) analysis of small molecules in complicated bio-samples. In this work, we presented a facile one-pot strategy for the synthesis of boric acid-functionalized covalent organic frameworks (B-COFs) by using 2, 4, 6-trihydroxy-1, 3, 5-benzenetrialdehyde, benzidine and 4-aminophenyl- boronic acid as ligands. Compared with bare COFs, the B-COFs have similar crystallinity, specific surface and well-developed pore structure. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b01376DOI Listing

Design and Performance of a Dual-Polarity Instrument for Ion Soft Landing.

Anal Chem 2019 Apr 19. Epub 2019 Apr 19.

A new apparatus for ion soft landing research was developed and is reported in this contribution. The instrument includes a dual polarity high flux electrospray ionization (ESI) interface, a tandem electrodynamic ion funnel system, a collisional flatapole, a quadrupole mass filter and a focusing lens. The instrument enables production of ionic layers by soft landing of mass-selected ions onto surfaces with balanced or imbalanced charge conditions using either layer-by-layer (LBL) or fast polarity switching modes. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00309DOI Listing

Magnetic Multiarm Scaffold for the One-step Purification of Epitope-Specific Neutralizing Antibodies.

Anal Chem 2019 Apr 18. Epub 2019 Apr 18.

Epitope-specific neutralizing antibodies (EsAbs) are of prime importance in the diagnosis and treatment of various serious diseases. However, obtaining EsAbs by the monoclonal antibody technique involves time-consuming and sophisticated multistep procedures, and the epitopes of the resulting antibodies are often not explicit. It is also very challenging to isolate EsAbs from numerous kinds of total immunoglobulins because of nonspecific adsorption and low separation efficiency. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00769DOI Listing

Maximizing Ion-tagged Oligonucleotide Loading on Magnetic Ionic Liquid Supports for the Sequence-Specific Extraction of Nucleic Acids.

Anal Chem 2019 Apr 17. Epub 2019 Apr 17.

Targeted nucleic acid analysis requires the highly selective extraction of desired DNA fragments in order to minimize interferences from samples with abundant heterogeneous sequences. We previously reported a method based on functionalized oligonucleotide probes known as ion-tagged oligonucleotides (ITOs) that hybridize with complementary DNA targets for subsequent capture using a hydrophobic magnetic ionic liquid (MIL) support. Although the ITO-MIL approach enriched specific DNA sequences in quantities comparable to a commercial magnetic bead-based method, the modest affinity of the ITO for the hydrophobic MIL limited the yield of DNA targets, particularly when stringent wash conditions were applied to remove untargeted DNA. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00350DOI Listing

The 2019 Reviews Issue.

Authors:
Robert T Kennedy

Anal Chem 2019 Jan;91(1)

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http://dx.doi.org/10.1021/acs.analchem.8b05701DOI Listing
January 2019

Controlled Release of Therapeutic Agents with NIR Laser for Synergistic Photo-Chemotherapy towards Cervical Cancer.

Anal Chem 2019 Apr 17. Epub 2019 Apr 17.

Different kinds of artificial drug delivery systems (DDS) have been widely exploited and utilized towards effective tumor therapy. Establishing a biocompatible DDS with a flexible release of the therapeutic agents has been one of the challenges and impetus to the development of tumor diagnosis and therapy fields. Herein, the chemotherapeutic agents doxorubicin hydrochloride (DOX) and photosensitizer indocyanine green (ICG) were simultaneously packaged into the cavity of Microvesicles (MVs) through electroporation technique. Read More

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http://dx.doi.org/10.1021/acs.analchem.8b05982DOI Listing

Ppb-level quartz-enhanced photoacoustic detection of carbon monoxide exploiting a surface grooved tuning fork.

Anal Chem 2019 Apr 17. Epub 2019 Apr 17.

A compact and sensitive carbon monoxide (CO) sensor was demonstrated by using quartz enhanced photoacoustic spec-troscopy (QEPAS) exploiting a novel 15.2 kHz quartz tuning fork (QTF) with grooved surfaces. The custom QTF was de-signed to provide a quality factor as high as 15,000 at atmospheric pressure, which offers a high detection sensitivity. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00182DOI Listing

Tri-component Multiblock Nanorods for Fourier Transform Surface Plasmon Resonance and its Chemical Sensing.

Anal Chem 2019 Apr 17. Epub 2019 Apr 17.

In this study, we report a new mode of chemical sensing using Fourier transform surface plasmon resonance with tri-component nanorods (Au, Ni and Pt). By applying an external magnetic field, magnetically responsive multi-block nanorods fluctuate periodically, producing sigmoidal optical responses that are represented as a dominant frequency peak after Fourier transform conversion. Adding H2O2 to the solution under an external magnetic field perturbed the periodic nanorod rotation due to a catalytic reaction between the Pt segment and H2O2, which produces catalytic random fluctuation states. Read More

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http://pubs.acs.org/doi/10.1021/acs.analchem.9b00466
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http://dx.doi.org/10.1021/acs.analchem.9b00466DOI Listing
April 2019
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Targeted Myocardial Hypoxia Imaging Using a Nitroreductase-Activatable Near-Infrared Fluorescent Nanoprobe.

Anal Chem 2019 Apr 17. Epub 2019 Apr 17.

Development of a highly selective and sensitive imaging probe for accurate detection of myocardial hypoxia will be helpful to estimate the degree of ischemia and subsequently guide personalized treatment. However, an efficient optical approach for hypoxia monitoring in myocardial ischemia is still lacking. In this work, a cardiomyocyte-specific and nitroreductase-activatable near-infrared nanoprobe has been developed for selective and sensitive imaging of myocardial hypoxia. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00298DOI Listing

Fluorescent chemosensor for dual-channel discrimination between phosgene and triphosgene.

Anal Chem 2019 Apr 17. Epub 2019 Apr 17.

As highly toxic and accessible chemical reagents, phosgene and triphosgene have become serious threat to public safety. So, it is highly desirable to develop facile methods to detect and recognize them. In this Article, a novel fluorescent chemosensor, Phos-4, has been constructed with 1,8-naphthalimide as the fluorophore and 2-(2-aminophenyl)imidazol as the recognition sites for discrimination between phosgene and triphosgene in dual-channel mode for the first time. Read More

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http://dx.doi.org/10.1021/acs.analchem.8b05777DOI Listing

The Interference Effect of Silica Colloidal Crystal Films and Their Applications on Biosensing.

Anal Chem 2019 Apr 17. Epub 2019 Apr 17.

With the aim to develop better and reliable interference effective substrates, silica colloidal crystal films with different sphere di-ameters and film thicknesses were successfully made by an improved vertical deposition method and a systematic investigation of their reflectometric interference spectroscopy (RIfS) properties was presented in this work. The influence of silica sphere diameter and film thickness on the RIfS signals was studied. Results showed that the film thickness is the key factor of RIfS signals. Read More

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http://pubs.acs.org/doi/10.1021/acs.analchem.9b00620
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http://dx.doi.org/10.1021/acs.analchem.9b00620DOI Listing
April 2019
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Design and demonstration of tunable amplified sensitivity of AlGaN/GaN high electron mobility transistor (HEMT)-based biosensors in human serum.

Anal Chem 2019 Apr 17. Epub 2019 Apr 17.

We have developed a swift and simplistic protein immunoassay using aptamer functionalized AlGaN/GaN high electron mobility transistors (HEMTs). The unique design of the sensor facilitates protein detection in physiological salt environment overcoming charge screening effects, without requiring sample pre-processing. This study reports a tunable and amplified sensitivity of solution-gated electric double layer (EDL) HEMT-based biosensors, which demonstrates significantly enhanced sensitivity by designing a smaller gap between the gate electrode and the detection, and by operating at higher gate voltage. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00353DOI Listing

A new platform for the direct profiling of microRNAs in biofluids.

Anal Chem 2019 Apr 17. Epub 2019 Apr 17.

Circulating microRNAs have been identified as potential biomarkers for early detection, prognosis and prediction of several diseases. Their use in clinical diagnostics has been limited by the lack of suitable detection techniques. Most of the current tech-nologies suffer from requiring complex protocols, not yet able to deliver robust and cost-effective assays in the field of clinical diagnostics. Read More

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http://pubs.acs.org/doi/10.1021/acs.analchem.9b00213
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http://dx.doi.org/10.1021/acs.analchem.9b00213DOI Listing
April 2019
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Ultrasensitive on-site detection of biological active ricin in complex food matrices based on immunomagnetic enrichment and fluorescence switch-on nanoprobe.

Anal Chem 2019 Apr 17. Epub 2019 Apr 17.

Ricin is a highly toxic protein largely existed in castor bean, which could be used as a warfare agent due to its unique properties. As a deadenylase, inactivation of ricin means loss of toxic threat. Therefore, developing simple, accurate and sensitive on-site detection of biologically active ricin in wide types of complex matrices is more valuable. Read More

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http://dx.doi.org/10.1021/acs.analchem.8b04458DOI Listing

Reducing the detrimental effects of saturation phenomena in FRET microscopy.

Anal Chem 2019 Apr 17. Epub 2019 Apr 17.

Although Förster resonance energy transfer (FRET) is one of the most widely used biophysical methods in biology, the effect of high excitation intensity, leading to donor and acceptor saturation, has not been addressed previously. Here, we present a formalism for the experimental determination of the FRET efficiency at high excitation intensity when saturation of both the donor and the acceptor significantly affect conventional FRET calculations. We show that the proposed methodology eliminates the dependence of the FRET efficiency on excitation intensity, which otherwise significantly distorts FRET calculations at high excitation intensities commonly used in experiments. Read More

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http://pubs.acs.org/doi/10.1021/acs.analchem.9b01504
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http://dx.doi.org/10.1021/acs.analchem.9b01504DOI Listing
April 2019
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Filter Beacon: A Gating-Free Architecture for Protein-Specific Glycoform Imaging on Cell Surface.

Anal Chem 2019 Apr 17. Epub 2019 Apr 17.

The imaging characterization of spatial proximity of covalently linked structural motifs (e.g., protein-specific glycoform) is essential for thorough understanding of cellular chemistry and biology. Read More

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http://pubs.acs.org/doi/10.1021/acs.analchem.9b00551
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http://dx.doi.org/10.1021/acs.analchem.9b00551DOI Listing
April 2019
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Identification of Vigilin as a potential ischemia biomarker by Brain Slice-based SELEX.

Anal Chem 2019 Apr 17. Epub 2019 Apr 17.

Cerebral stroke is the leading cause of disability and death among adults worldwide, and results in numerous biochemical alterations. However, few efficient biomarkers are clinically available to diagnose cerebral stroke because of the limitations of biomarkers and their probes. In this work, we utilized frozen brain slices of middle cerebral artery occlusion (MCAO) in a mouse model of ischemia to select a specific binding aptamer, termed LCW17, by tissue-based SELEX (systematic evolution of ligands by exponential enrichment). Read More

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http://pubs.acs.org/doi/10.1021/acs.analchem.9b00609
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http://dx.doi.org/10.1021/acs.analchem.9b00609DOI Listing
April 2019
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MS-Based Molecular Networking of Designer Drugs as an Approach for the Detection of Unknown Derivatives for Forensic and Doping Applications: A Case of NBOMe Derivatives.

Anal Chem 2019 Apr 18. Epub 2019 Apr 18.

Institute of Pharmaceutical Science and Technology and College of Pharmacy , Hanyang University , Ansan , Gyeonggi-do 15588 , Republic of Korea.

The NBOMe family is a group of new psychoactive substances (NPSs). In this study, the fragmentation patterns of NBOMe derivatives were analyzed using liquid chromatography quadrupole time-of-flight mass spectrometry (LC-QTOF/MS). The MS/MS spectral data was used to establish a molecular networking map for NBOMe derivatives. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00294DOI Listing

Deep MS/MS-Aided Structural-similarity Scoring for Unknown Metabolites Identification.

Anal Chem 2019 Apr 16. Epub 2019 Apr 16.

Tandem mass spectrometry (MS/MS) is the workhorse for structural annotation of metabolites, because it can provide abundance of structural information. Currently, metabolite identification mainly relies on querying experimental spectra against public or in-house spectral databases. The identification is severely limited by the available spectra in the databases. Read More

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http://dx.doi.org/10.1021/acs.analchem.8b05405DOI Listing

Three-Dimensional NMR Spectroscopy of Fluorinated Pharmaceutical Solids under Ultrafast Magic Angle Spinning.

Anal Chem 2019 Apr 16. Epub 2019 Apr 16.

High-resolution solid-state analysis of multicomponent molecular systems, e.g., pharmaceutical formulations, is a great challenge. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00884DOI Listing

Surface-Enhanced Raman Scattering Probing the Translocation of DNA and Amino Acid through Plasmonic Nanopores.

Anal Chem 2019 Apr 16. Epub 2019 Apr 16.

DNA and amino acid are important biomolecules in living organism. Probing such biomolecules with structural characters can provide valuable information for life study. Here, gold plasmonic nanopores (GPNs) with high SERS activity (a local enhancement factor higher than 10) are synthesized at the tip of a glass nanopipette. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b01045DOI Listing

A Proteomic Strategy for Identification of Proteins Responding to Cisplatin-Damaged DNA.

Anal Chem 2019 Apr 16. Epub 2019 Apr 16.

A new proteomic strategy combining functionalized magnetic nanoparticle affinity probes with mass spectrometry was developed to capture and identify proteins specifically responding to 1,2-d(GpG) intrastrand cisplatin-crosslinked DNA, the major DNA lesion caused by cisplatin and thought to induce apoptosis. A 16-mer oligodeoxynucleotide (ODN) duplex and its cisplatin-crosslinked adduct were immobilized on magnetic nanoparticles via click reaction, respectively, to fabricate negative and positive affinity probes which were very stable in cellular protein extracts due to the excellent bio-orthogonality of click chemistry and the inertness of covalent triazole linker. Quantitative mass spectrometry results unambiguously revealed the predominant binding of HMGB1 and HMGB2, the well-established specific binders of 1,2-cisplatin-crosslinked DNA, to the cisplatin-crosslinked ODN, thus validating the accuracy and reliability of our strategy. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00554DOI Listing

AuNCs-Catalyzed Hydrogen Selenide Oxidation: Mechanism and Application for Headspace Fluorescent Detection of Se(IV).

Anal Chem 2019 Apr 16. Epub 2019 Apr 16.

The excellent fluorescence property of Au nanoclusters (AuNCs) has received great attention for various chemosensing and bio-related applications, but the sample matrix is still a cursing problem that causes undesirable fluorescence variation. Hydride generation (HG) is an effective strategy to separate the target analyte from the complex sample matrices, but the implementation of HG with AuNC-based fluorescent assays was not realized. On the other hand, due to the ultrasmall size of AuNCs and good catalytic performance of Au, AuNCs are also featuring intriguing catalytic applications. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00738DOI Listing

A Ratiometric Fluorescent Probe for Monitoring Endogenous Methylglyoxal in Living Cells and Diabetic Blood Samples.

Anal Chem 2019 Apr 16. Epub 2019 Apr 16.

Optical imaging provides noninvasive powerful tools not only for better understanding the physiological and pathological roles of Methylglyoxal (MGO) in living systems but also for potential clinical diagnosis of MGO-related diseases such as diabetic complications. However, so far only very few "turn-on" MGO fluorescent sensors have been developed, and they are all based on the reaction between MGO and benzenediamines. Due to the possible reactions of benzenediamines with other cellular molecules such as NO and FA, these sensors suffer from limited selectivity and potential deactivation in cells. Read More

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http://dx.doi.org/10.1021/acs.analchem.8b05426DOI Listing
April 2019
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Differentiation of Intracellular Hyaluronidase Isoform by Degradable Nanoassembly Coupled with RNA-Binding Fluorescence Amplification.

Anal Chem 2019 Apr 16. Epub 2019 Apr 16.

Hyaluronidase has two cruical isoforms, hyaluronidase-1 (Hyal-1) and hyaluronidase-2 (Hyal-2), which are essential for cellular hyaluronic acid (HA) catabolism to generate different-sized oligosaccharide fragments for performing different physiological functions. In particular, Hyal-1 is the major tumor-derived hyaluronidase. Thus, specific detection of one hyaluronidase isoform, especially Hyal-1, in live cells is of scientific significance but remains challenging. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b01242DOI Listing

Direct Blue Light-induced Autocatalytic Oxidation of o-Phenylenediamine for Highly Sensitive Visual Detection of Triaminotrinitrobenzene.

Anal Chem 2019 Apr 16. Epub 2019 Apr 16.

o-Phenylenediamine (OPD)-based chromogenic reactions are worthy tools for development of visual colorimetric assays. The chromogenic reactions are usually triggered by various oxidants, which is not easily tunable and incompatible with some analytes. Herein, we report that direct blue light irradiation can induce the autocatalytic oxidation of OPD to generate 2,3-diaminophenazine (oxidized-state OPD, oxOPD). Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00759DOI Listing

Enhanced visual wireless electrochemiluminescence immunosensing of prostate-specific antigen based on the luminol loaded into MIL-53(Fe)-NH2 accelerator and hydrogen evolution reaction mediation.

Anal Chem 2019 Apr 16. Epub 2019 Apr 16.

A sensitive PSA detection method using a visual-readout closed bipolar electrode (BPE) system has been introduced by integration of hydrogen evolution reaction (HER) in cathodic pole and electrochemiluminescence (ECL) of luminol-loaded with-in the MIL-53(Fe)-NH2 (L@MIL-53(Fe)-NH2) in the anodic pole. The cathode of the BPE was electrochemically synthesized by 3D porous copper foam, followed by decorating with nitrogen-doped graphene nanosheet and ruthenium nanoparticles. The alternative, we employed carboxylate-modified magnetic nanoparticles (MNPs) for immobilization of the primary antibody (Ab1) and utilized the L@MIL-53(Fe)-NH2 conjugated to secondary antibody (Ab2) as a signaling probe and co-reaction accelerator. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b01506DOI Listing

Photoelectrochemical imaging system for the mapping of cell surface charges.

Anal Chem 2019 Apr 15. Epub 2019 Apr 15.

The surface charge of cells affects cell signaling, cell metabolic processes, adherence to surfaces and cell proliferation. Our understanding of the role of membrane charges is limited due to the inability to observe changes without interfering, chemically or physically, with the cell or its membrane. Here, we report that a photoelectrochemical imaging system (PEIS) based on label-free ac-photocurrent measurements at indium tin oxide (ITO) coated glass substrates can be used to map the basal surface charge of single live cells under physiological conditions. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00304DOI Listing

Nonlinear spectroscopy reveals how external pH controls permeation and accumulation of small molecules in two cellular compartments of Escherichia coli.

Anal Chem 2019 Apr 15. Epub 2019 Apr 15.

Quantitative evaluation of small molecule permeation and accumulation in Gram-negative bacteria is important for drug development against them. While these measurements are commonly performed at physiological pH, Escherichia coli and many other Enterobacteriaceae infect human gastrointestinal and urinary tracts where they encounter different pH conditions. To understand how external pH affects permeation and accumulation of small molecules in E. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00574DOI Listing

Optomechanical Time-Gated Fluorescence Imaging Using Long-Lived Silicon Quantum Dot Nanoparticles.

Anal Chem 2019 Apr 17. Epub 2019 Apr 17.

University of Michigan-Shanghai Jiao Tong University Joint Institute , Shanghai Jiao Tong University , Shanghai 200240 , China.

We demonstrate a novel optomechanical synchronization method to achieve ultrahigh-contrast time-gated fluorescence imaging using live zebrafish as models. Silicon quantum dot nanoparticles (SiQDNPs) with photoluminescence lifetime of about 16 μs were used as the long-lived probes to enable background autofluorescence removal and multiplexing through time-gating. A continuous-wave 405 nm laser as the excitation source was focused on a rotating optical chopper on which the emission light beam obtained from an inverted fluorescence microscope was also focused but with a phase difference such that in a short delay after the excitation laser is blocked, the emission light beam passes through the optical chopper, initiating the image acquisition by a conventional sensor. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00517DOI Listing
April 2019
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Evaluation of distance metrics and spatial autocorrelation in Uniform Manifold Approximation and Projection applied to Mass Spectrometry Imaging data.

Anal Chem 2019 Apr 15. Epub 2019 Apr 15.

In this work Uniform Manifold Approximation and Projection (UMAP) is applied for non-linear dimensionality reduction and visualisation of Mass Spectrometry Imaging (MSI) data. We evaluate the performance of the UMAP algorithm on MSI datasets acquired in mouse pancreas and human lymphoma samples and compare it to those of principal component analysis (PCA), t-distributed Stochastic Neighbour Embedding (t-SNE) and the Barnes-Hut (BH) approximation thereof. Furthermore, we compare different distance metrics in (BH) t-SNE and UMAP, and propose the use of spatial autocorrelation as a means of comparing the resulting low-dimensional embeddings. Read More

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http://dx.doi.org/10.1021/acs.analchem.8b05827DOI Listing
April 2019
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Metal-Organic Framework Enhances Aggregation-Induced Fluorescence of Chlortetracycline and the Application for Detection.

Anal Chem 2019 Apr 15. Epub 2019 Apr 15.

The development of analytical method for selective and sensitive detection of chlortetracycline (CTC), an often over-used broad spectrum antibiotic, is important and challenging in environmental and health monitoring. This paper reports a zinc based metal-organic framework of pyromellitic acid (Zn-BTEC), which has been found to greatly enhance the aggregation-induced emission (AIE) of chlortetracycline. The unique emission response of CTC on Zn-BTEC has been extensively examined and applied for the sensitive detection of CTC on the basis of fluorescence intensity of AIE, and a limit of detection (LOD) was estimated to be 28 nM. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00319DOI Listing

Micromotor-Assisted Human Serum Glucose Biosensing.

Anal Chem 2019 Apr 15. Epub 2019 Apr 15.

Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences , Nanyang Technological University , Singapore 637371 , Singapore.

Artificial self-propelled micromachines have shown great promise in biomedical sciences. In this work, we use Mg/Pt Janus micromotors with self-rejuvenating surfaces to enhance the electrochemical sensing performance and sensitivity toward glucose in human serum. The detection of glucose is based on the glucose oxidase enzyme and ferrocenemethanol shuttle system, where mass transfer was dramatically enhanced by the rapid motion of Mg/Pt Janus micromotors. Read More

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http://dx.doi.org/10.1021/acs.analchem.8b05464DOI Listing

Phenotype Profiling for Forensic Purposes: Determining Donor Sex based on Fourier Transform Infrared Spectroscopy of Urine Traces.

Anal Chem 2019 Apr 15. Epub 2019 Apr 15.

Forensic science is an important field of analytical chemistry where vibrational spectroscopy, in particular Fourier transform infrared spectroscopy and Raman spectroscopy, present advantages as they have a non-destructive nature, high selectivity, and no need for sample preparation. Herein, we demonstrate a novel method for determination of donor sex, based on attenuated total reflection Fourier transform infrared (ATR FT-IR) spectroscopy of dry urine traces. Trace body fluid evidence is of special importance to the modern criminal investigation as a source of individualizing DNA evidence. Read More

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http://pubs.acs.org/doi/10.1021/acs.analchem.9b01058
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http://dx.doi.org/10.1021/acs.analchem.9b01058DOI Listing
April 2019
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Reaction monitoring using SABRE-hyperpolarized benchtop (1 T) NMR spectroscopy.

Anal Chem 2019 Apr 15. Epub 2019 Apr 15.

The conversion of [IrCl(COD)(IMes)] (COD = cis,cis-1,5-cyclooctadiene, IMes = 1,3-bis(2,4,6-trimethyl-phenyl)imidazole-2-ylidene) in the presence of an excess of p-H and a substrate (4-aminopyridine (4-AP) or 4-methylpyridine (4-MP)) into [Ir(H)(IMes)(substrate)]Cl is monitored by H NMR spectroscopy using a benchtop (1 T) spectrometer in conjunction with the parahydrogen (p-H) based hyperpolarization technique signal amplification by reversible exchange (SABRE). A series of single-shot H NMR measurements are also used in parallel to monitor these chemical changes that take place in solution through the life-time of the hyperpolarized response. Non-hyperpolarized high-field H NMR control measurements were also undertaken to confirm that the observed time dependent changes relate directly to the underlying chemical evolution. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00729DOI Listing

Smartphone Nano-Colorimetric Determination of Hydrogen Sulfide in Biosamples After Silver-Gold Core-Shell Nanoprism-Based Headspace Single-Drop Microextraction.

Anal Chem 2019 Apr 15. Epub 2019 Apr 15.

In this work, sensitive detection of hydrogen sulfide (H2S) was realized at low cost and high efficiency through the application of silver-gold core-shell nanoprism (Ag@Au-np) combined with headspace-single drop microextraction (HS-SDME). After SDME, smartphone nano-colorimetry (SNC), with the aid of a smartphone camera and a colour picker software, was used to detect and quantify the H2S. The method took advantage of the inhibition of the ultraviolet-visible (UV-vis) signal caused by H2S etching of the Ag@Au-np pre-added to the SDME solvent, to measure the H2S concentration. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00255DOI Listing

A Strategy for Structural Elucidation of Polysaccharides: Elucidation of a Maize Mucilage that Harbors Diazotrophic Bacteria.

Anal Chem 2019 Apr 15. Epub 2019 Apr 15.

Polysaccharides are the most abundant biomolecule in nature and are ubiquitously found in every kingdom of life. Despite their natural abundance, methods for the characterization of their complicated structures have lagged behind both proteins and DNA. Polysaccharides can reach up to one million daltons and may contain many different monosaccharides, glycosidic linkages, and branching patterns, all of which add additional analytical challenges. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00789DOI Listing

Supercritical fluid chromatography on-chip with two-photon excited fluorescence detection for high-speed chiral separations.

Anal Chem 2019 Apr 15. Epub 2019 Apr 15.

Herein we present the first example of microchip-based supercritical fluid chromatography (SFC). A glass microfluidic plat-form with pressure and temperature control for fast and efficient on-column injection is described. This enabled fast and efficient separation of chiral compounds within seconds employing also two-photon excitation fluorescence detection. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00726DOI Listing

Comprehensive Characterization of Biotherapeutics by Selective Capturing of Highly Acidic Glycans using Stepwise PGC-SPE and LC/MS/MS.

Anal Chem 2019 Apr 15. Epub 2019 Apr 15.

The glycosylation of biologics is an important factor in pharmacological functions such as efficacy, safety, and biological activity and is easily affected by subtle changes in the cellular environment. Hence, comprehensive and in-depth glycomic characterization of biological products should be performed to ensure product quality and process consistency prior to regulatory approval, but it is still highly challenging due to glycan micro-heterogeneity produced by enzymatic machinery. In this study, we have developed a systematic methodology for the separation and characterization of various glycans of biotherapeutics using the combination of solid phase extraction (SPE) and high resolution LC/MS. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00603DOI Listing

Highly Sensitive O-Glycan Profiling for Human Serum Proteins Reveals Gender-Dependent Changes in Colorectal Cancer Patients.

Anal Chem 2019 Apr 15. Epub 2019 Apr 15.

A newly developed microscale protocol for profiling serum O-glycans has been validated here with multiple serum samples obtained from different cohorts of colorectal cancer patients. The simultaneous cleavage and permethylation steps in this procedure preserve the integrity of released minor O-glycans, so that 39 O-linked oligosaccharides could be reliably recorded in a profile. This is far more detected components than shown in any previous studies. Read More

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http://dx.doi.org/10.1021/acs.analchem.9b00822DOI Listing