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Despite the great potential of microplasma optical emission spectrometry (OES) for on-site analysis, it remains a challenge to achieve the fast, sensitive, batch, and multielement analysis of trace heavy metals in a complex matrix. Herein, a novel ultrasonic nebulization-accelerated gas-phase enrichment (GPE) following in situ microplasma desorption sampling approach is employed for the determination of trace heavy metals by a miniature dielectric barrier discharge (DBD)-OES device. The volatile heavy metal species obtained by hydride generation (HG) can be quickly separated from the complex matrix under the action of ultrasonic nebulization, adsorbed on the surface of the activated carbon electrode tip for GPE, and then in situ desorbed and excited by DBD microplasma to achieve multielement OES analysis. With an array nebulizer plate, a batch of 10 samples can be handled for GPE in 40 s, and DBD-OES analysis is maintained at a rate of 6 s per sample. Under the optimized conditions, the detection limits for simultaneous determinations of Hg, Cd, Cu, and Sn are 0.005, 0.01, 0.03, and 0.04 μg L

Point-of-care testing (POCT) with the advantages of simplicity, rapidity, portability, and low-cost is of great importance to improve healthcare, especially in resource-limited settings and home healthcare settings. Moreover, it is a great challenge to quantitative POCT of multiplexed biomarkers within a single accessible assay but provides enhanced diagnostic accuracy and improved diagnostic efficiency. Herein, a smartphone optical device has been designed for POCT of glucose and cholesterol in metabolic syndrome patients using a ratiometric fluorescent sensor. The sensing system of Ag NPs/UiO-66-NH2 and o-phenylenediamine presents a dual-emission response to H2O2 (the main product of glucose and cholesterol catalyzed by glucose oxidase and cholesterol oxidase) on account of the inner filter effect, resulting in an increase in the response of the fluorescence intensity ratio (F555 nm/F425 nm) accompanied by a distinguishable color transition from blue to yellow green. After compositing probes with a flexible substrate, the obtained test strip can be integrated with a smartphone-based portable platform to read RGB values for accurate testing of glucose and cholesterol with both detection limits of 10 μmol L-1, which are hundreds of times lower than their concentrations in human serum. With the advantages of low-cost, ease of operation, and broad adaptability, this smartphone optical device holds great potential for portable detection of numerous targets in personalized healthcare and clinical diagnosis.

Quantification of exosomal multi-miRNA can reveal the initiation, progression, and metastasis of tumors, which is conducive to the noninvasive early diagnosis of cancer. However, low-sensitivity and single-plex detection characteristics of traditional methods seriously hinder the accuracy and specificity of exosomal miRNAs in cancer diagnosis. Herein, we design an ultramultiplexing strategy that enables simultaneous and sensitive detection of multiple exosomal miRNAs by nanosatellites (magnetic beads (MBs) @ NaLnF

Azodicarbonamide (ADA) is widely used as a flour additive due to its oxidizing and bleaching properties, but it reacts with wet flour during heat processing and is easily decomposed into semicarbazide with genotoxicity and carcinogenicity. In order to improve the efficiency of food safety supervision and expand the scope of food safety control, it is of great significance to develop a facile method for point-of-care testing (POCT) of ADA. Herein, a field-portable and universal smartphone-based photoacoustic (PA) integration device is constructed for quantitative POCT of ADA in flour. The recognition probe Prussian blue with favorable stability is loaded on a flexible substrate for fabricating a portable test strip. In the presence of target ADA, the PA signal changes driven by a modulated 808 nm laser beam can be conveniently collected through the recording application (Audio Lab) of the smartphone. By combining the economic test strip and portable PA device with smartphone readout, it not only greatly simplifies the operation steps but also dramatically reduces the size and cost of the instrument. There is a favorable linear relationship between the PA signal and ADA concentration in the range of 10-200 μmol L

Speciation analysis of arsenic in blood is essential for identifying and quantifying the exposure of arsenic and studying the metabolism and toxicity of arsenic. Herein, a novel pretreatment device is rationally designed and used for speciation analysis of arsenic in whole blood by ion chromatography-inductively coupled plasma-mass spectrometry (IC-ICP-MS). The sample centrifuge tubes containing blood, reagents, and a magnetic stir bar are placed on the fidget spinner of the pretreatment device. When flicking the fidget spinner rotation with the finger, the magnetic stir bar in the tube rotates in three dimensions under the magnetic field, thereby assisting dispersive extraction of arsenic species by the mixing of blood with reagents. Afterward, the arsenic extract is separated in situ from the blood matrix using an ultrasonic spray sheet covered with a filter and ultrafiltration membrane, which is directly used for subsequent IC-ICP-MS analysis. For 100 μL of blood, the whole pretreatment operation can be completed within 10 min. With As(III), As(V), MMA, and DMA in blood as analytes, the use of the present pretreatment device will hardly lead to the loss and transformation of arsenic species, and the extraction efficiency of the total arsenic is more than 96%. When the pretreatment device is coupled to IC-ICP-MS, the detection limits of four arsenic species in whole blood are 0.017-0.023 μg L-1, and precisions are within 2.3-4.2%. This pretreatment device provides a simple, fast, efficient, and low-cost tool for extraction and separation of arsenic species in whole blood, opening a new idea for the pretreatment of complex samples.

Tumor exosomes with molecular marker-proteins inherited from their parent cells have emerged as a promising liquid biopsy biomarker for cancer diagnosis. However, facile, robust, and sensitive detection of exosomal proteins remains challenging. Therefore, a nanozyme sensor array is constructed by using aptamer-modified C3N4 nanosheets (Apt/C3N4 NSs) together with a solvent-mediated signal amplification strategy for ratiometric fluorescence detection of exosomal proteins. Three aptamers specific to exosomal proteins are selected to construct Apt/C3N4 NSs for high specific recognition of exosomal proteins. The adsorption of aptamers enhances the catalytic activity of C3N4 NSs as a nanozyme for oxidation of o-phenylenediamine (oPD) to 2,3-diaminophenazine (DAP). In the presence of target exosomes, the strong affinity between aptamer and exosome leads to the disintegration of Apt/C3N4 NSs, resulting in a decrease of catalytic activity, thereby reducing the production of DAP. The ratiometric fluorescence signal based on a photoinduced electron transfer (PET) effect between DAP and C3N4 NSs is dependent on the concentration of DAP generated, thus achieving highly facile and robust detection of exosomal proteins. Remarkably, the addition of organic solvent-1,4-dioxane can sensitize the luminescence of DAP without affecting the intrinsic fluorescence of C3N4 NSs, achieving the amplification of the aptamer-exosome recognition events. The detection limit for exosome is 2.5 × 103 particles/mL. In addition, the accurate identification of cancer can be achieved by machine learning algorithms to analyze the difference of exosomal proteins from different patients' blood. We hope that this facile, robust, sensitive, and versatile nanozyme sensor array would become a promising tool in the field of cancer diagnosis.

Exosomes are expected to be used as cancer biomarkers because they carry a variety of cancer-related proteins inherited from parental cells. However, it is still challenging to develop a sensitive, robust, and high-throughput technique for simultaneous detection of exosomal proteins. Herein, three aptamers specific to cancer-associated proteins (CD63, EpCAM, and HER2) are selected to connect gold nanoparticles (AuNPs) as core with three different elements (Y, Eu, and Tb) doped up-conversion nanoparticles (UCNPs) as satellites, thereby forming three nanosatellite assemblies. The presence of exosomes causes specific aptamers to recognize surface proteins and release the corresponding UCNPs, which can be simultaneously detected by inductively coupled plasma-mass spectrometry (ICP-MS). It is worth noting that rare earth elements are scarcely present in living systems, which minimize the background for ICP-MS detection and exclude potential interferences from the coexisting species. Using this method, we are able to simultaneously detect three exosomal proteins within 40 min, and the limit of detection for exosome is 4.7 × 103 particles/mL. The exosomes from seven different cell lines (L-02, HepG2, GES-1, MGC803, AGS, HeLa, and MCF-7) can be distinguished with 100% accuracy by linear discriminant analysis. In addition, this analytical strategy is successfully used to detect exosomes in clinical samples to distinguish stomach cancer patients from healthy individuals. These results suggest that this sensitive and high-throughput analytical strategy based on ICP-MS has the potential to play an important role in the detection of multiple exosomal proteins and the identification of early cancer.

The miniaturized optical emission spectrometry (OES) devices based on various microplasma excitation sources provide reliable tools for on-site analysis of heavy metal pollution, while the development of convenient and efficient sample introduction approaches is essential to improve their performances for field analysis. Herein, a small activated carbon electrode tip is employed as solid support to preconcentrate heavy metals in water and subsequently served as an inner electrode of the coaxial dielectric barrier discharge (DBD) to generate microplasma. In this case, heavy metal analytes in water are first adsorbed on the surface of the activated carbon electrode tip via a simple liquid-solid phase transformation during the sample loading process, and then, fast released to produce OES during the DBD microplasma excitation process. The corresponding OES signals are synchronously recorded by a charge-coupled device (CCD) spectrometer for quantitative analysis. This activated carbon electrode tip provides a new tool for sample introduction into the DBD microplasma and facilitates "insert-and-go" in subsequent DBD-OES analysis. With a multiplexed activated carbon electrode tip array, a batch of water samples (50 mL) can be loaded in parallel within 5 min. After drying the activated carbon electrode tips for 5 min, the DBD-OES analysis is maintained at a rate of 6 s per sample. Under the optimized conditions, the detection limits of 0.03 and 0.6 μg L-1 are obtained for Cd and Pb, respectively. The accuracy and practicability of the present DBD-OES system have been verified by measuring several certified reference materials and real water samples. This analytical strategy not only simplifies the sample pretreatment steps but also significantly improves the sensitivity of the DBD-OES system for heavy metal detection. By virtue of the advantages of high sensitivity, fast analysis speed, simple operation, low cost, and favorable portability, the upgraded DBD-OES system provides a more powerful tool for on-site analysis of heavy metal pollution.

Lipid droplets (LDs) are intracellular lipid-rich organelles, which not only serve as neutral lipid reservoirs but also involve in many physiological processes and are associated with a variety of metabolic diseases and cancers. Long-term tracking of the state and behavior of LDs is of great significance but challenging. The difficulty is largely due to the lack of low cytotoxicity, high photobleaching resistance, and long intracellular retention probes that are capable of long-term tracking LDs. Herein, we report the discovery of two amphiphilic LD-targeting carbon nanoparticles (CNPs, i.e., CPDs and CDs) prepared by one-step room-temperature and hydrothermal methods. Their high lipid-water partition coefficient (log P > 2.13) and strong positive solvatochromism property ensure the quality of LD imaging. Especially, CDs exhibit favorable biocompatibility (2 mg mL-1, cell viability >90%), excellent photostability (after continuous laser irradiation on a confocal microscope for 2 h, relative FL intensity >85%), and superior intracellular retention ability, thereby enabling long-term tracking of LDs in hepatocytes for up to six passages. Based on the excellent long-term tracking ability, CDs are successfully applied to observe autophagy in a typical catabolic process and to evaluate the effect of a commonly used lipid-lowering drug atorvastatin on hepatocyte lipid uptake.

Butyrylcholinesterase (BuChE), the primary source of serum cholinesterase activity, is an indispensable biochemical marker for clinical diagnosis of liver function and organophosphorus poisoning. The requirement for bulky and expensive instruments represents a huge hindrance for point-of-care testing (POCT) of BuChE, especially in resource-limited settings. Herein, an easy-operated, economic, and portable photothermal (PT) biosensing platform for high-throughput BuChE detection was rationally designed. BuChE could "light up" the PT signal through in situ generation of Prussian blue (PB) by MIL-53 (Fe), which allowed us to translate biological signals into temperature signals. Such temperature change signals could be monitored at high throughput (six samples for a single measurement) by a miniature self-made integrated PT device via combining separable 96-well plates, a three-dimensional (3D) printed sample bracket, 808 nm lasers, and thermometers, satisfying the requirement for rapid on-site detection in a large batch with low cost. In addition, the large specific surface area, 3D network structure, and high porosity of MIL-53 (Fe) offered a beneficial platform for its reaction with enzymatic hydrolysate, resulting in high sensing sensitivity and low detection limit (0.3 U L-1), which was at least 20 000 times lower than the normal human serum BuChE activity. This facile, affordable, and broad applicability PT sensing platform provides a beneficial reference for the rational design of other disease diagnostic approaches suitable for POCT.

A microplasma-based optical emission spectrometry (OES) system has emerged as a potential tool for field analysis of heavy metal pollution due to its features of portability and low energy consumption, while the development of an efficient sample introduction approach against matrix interference is crucial to meet the requirements of complex sample analysis. Herein, a MoS

Single-cell-based genomics and transcriptomics analysis have revealed substantial cellular heterogeneity among seemingly identical cells. Knowledge of the cellular heterogeneity at multiomics levels is vital for a better understanding of tumor metastasis and drug resistance, stem cell differentiation, and embryonic development. However, unlike genomics and transcriptomics studies, single-cell characterization of metabolites, proteins, and post-translational modifications at the omics level remains challenging due to the lack of amplification methods and the wide diversity of these biomolecules. Therefore, new tools that are capable of investigating these unamplifiable "omes" from the same single cells are in high demand. In this work, a microwell chip was prepared and the internal surface was modified for hydrophilic interaction liquid chromatography-based tandem extraction of metabolites and proteins and subsequent protein digestion. Next, direct electrospray ionization mass spectrometry was adopted for single-cell metabolome identification, and a data-independent acquisition-mass spectrometry approach was established for simultaneous proteome profiling and phosphoproteome analysis without phosphopeptide enrichment. This integrated strategy resulted in 132 putatively annotated compounds, more than 1200 proteins, and the first large-scale phosphorylation data set from single-cell analysis. Application of this strategy in chemical perturbation studies provides a multiomics view of cellular changes, demonstrating its capability for more comprehensive investigation of cellular heterogeneity.

A two-dimensional cytometry platform (CytoLM) with high sensitivity and high temporal resolution is developed for single-particle and single-cell sampling and analysis. First, a Dean flow-assisted vortex capillary cell sampling (VCCS) unit confines the sample stream in curved flow and drives to focus and align the particles or cells in a small probe volume. By coupling VCCS to a laser-induced fluorescence (LIF) detector with data acquisition and processing capability, a high-throughput single-particle/cell analysis system (VCCS-LIF) was established. The particle analysis throughput of 119.42/s and a detection recovery of 78.20 ± 1.75% were achieved at a density of 9.16 × 104/mL for fluorescent particles, and the cell analysis throughput is 48.20/s at a density of 1.5 × 105/mL. Second, the CytoLM platform is constructed by hyphenating VCCS-LIF with inductively coupled plasma mass spectrometry (ICP-MS). In the analysis of HepG2 cells by Ag+ incubation and AO staining, 10,760 fluorescence bursts and 3068 MS events were observed in 240 s. Invalid signals due to undispersed cells were controlled at 3.80% for LIF and 1.01% for MS, with a proportion of effective signal of >96.20%. After peak identification and integral processing of the original data, the statistical results including peak area, height, width, and spacing are obtained concurrently and the information on concentration and elemental quantification of single cells is evaluated. CytoLM facilitates high-throughput, multi-dimensional, and multi-parameter characterization of particles and cells, and it may provide vast potential in life science analysis.

The discrimination of various sulfur -containing species helps us to deeply understand how sulfur affects cellular signaling and other physiological events. Herein, we present a three-dimensional sensor array based on simultaneous variation of the optical properties (fluorescence, light scattering, and UV–vis absorption) of gold–silver alloy nanocluster (AuAgNCs)–gold nanoparticle (AuNPs) composite for the rapid identification of 13 sulfur-containing species and sulfur-oxidizing bacteria. The sensor array is fabricated based on the strong coordination interactions between sulfur-containing compounds and AuAgNCs on the surface of AuNPs. The sulfur species of interest exhibit different affinities toward AuAgNCs and generate unique optical properties. These response patterns could divide the analytes into three categories including organic sulfide, inorganic sulfide, and thiols. Thirteen types of sulfur species including cystine, methionine, GSSG, S2–, SO32–, S2O32–, S2O72–, S2O82–, S4O62–, GSH, N-acetyl-l-c...

In view of the high toxicity of Cr(VI), simple and rapid on-site analytical approaches are in high demand for environment monitoring. Herein, an innovative chemosensor is developed for on-site sensitive detection of Cr(VI) in minutes by the naked eye. The chemosensor consists of gallic acid-capped gold nanoparticles (GA-Au NPs), methylene blue (MB), and NaBH4. In the presence of Cr(VI) ions, the reduction of MB by NaBH4 is able to greatly accelerate due to the Cr(VI)-stimulated catalytic activity of GA-Au NPs, resulting in a color switching of MB from blue to colorless for the quantitative detection of Cr(VI). The chemosensor in solution exhibits excellent selectivity and ultrahigh sensitivity to Cr(VI), with the detection limits of 0.05 nM by UV-vis spectroscopy and 0.1 nM by the naked eye. Similarly, a paper-based chemosensor is obtained by immobilization of GA-Au NPs and MB onto a piece of filter paper, offering a more convenient approach for rapid on-site detection of Cr(VI). In addition, H2O2 as an oxidizing agent is employed to convert Cr(III) into Cr(VI), thus achieving speciation analysis of Cr. The applicability of a chemosensor is also validated by the detection of Cr speciation in water samples with satisfactory recoveries.

Fluorescence imaging of cellular metals is widely reported. However, the quantification of intracellular metals with fluorescence imaging is so far not feasible and highly challenging. In this work, a ratiometric probe with two fluorescently labeled complementary DNA strains is designed for intracellular zinc quantification via fluorescence imaging, based on fluorescence resonance energy transfer (FRET) from carbon dots (CDs) to fluorescein (FAM). The donor CDs are modified with a Zn2+ aptamer, whereas the receptor FAM is conjugated with the complementary DNA sequence to ensure selectivity. MCF-7 cells are cultured sequentially with Zn2+ (20, 40, 55, 70, 85, and 100 μmol L–1) and CDs–FAM (100 μg mL–1), which is used for fluorescence imaging (at λex = 405 nm and λem = 440–490 nm for CDs, λem = 500–550 nm for FAM) to provide a relative fluorescence ratio ((F – F0)/F0, F = ICDs/IFAM), followed by quantifying intracellular zinc with ICPMS. A linear correlation is achieved between the relative fluorescence rat...

Real-time and rapid detection of various biomarkers in body fluids has important significance for early disease diagnosis, efficient monitoring of treatment, and evaluation of prognosis. However, traditional detection methods not only require bulky and costly instruments but also are not suitable for the analysis of heterogeneous samples (e.g., serum and urine), limiting their applications in point-of-care testing (POCT). Herein, an integrated photoacoustic (PA) device with a smartphone as the acoustic signal readout has been constructed, greatly reducing the volume and cost of the instrument, and providing a potential miniature platform for POCT of clinical samples. By exploiting the electron transfer product of 3,3',5,5'-tetramethylbenzidine (TMB) (i.e., TMB++) as the PA probe and hemin-graphene oxide (H-GO) complex as the peroxidase, quantitative analysis of uric acid was successfully performed by using only 30 μL of a sample solution. Due to the favorable stability of artificial enzymes, reaction reagents could be effectively embedded in agar gel to make a portable "test strip". Therefore, operators just need to drop clinical samples on the "test strip" for PA analysis, which is user friendly without requiring complex sample preparation steps. In addition, since the acoustic change mainly comes from the PA effect, it has a lower background signal than UV-vis and fluorescence analysis, greatly improving the analytical performance. The simplicity, low cost, and broad adaptability make this miniature PA device attractive for on-site detection, particularly in resource-limited settings.

Systematically tuning the structures and properties of noble-metal nanoparticles through biomolecule-mediated overgrowth is of significant importance for their applications in biosensing and imaging. Herein thiolated biomolecules with different concentrations and sizes (molecular weight and spatial structure) were used as a class of capping ligands to control the longitudinal surface plasmon resonance (LSPR) property of gold nanorods (GNRs). The LSPR peaks were red-shifted by increasing the capping agent concentration. The size effect could be divided to two aspects: (1) When the ligands are small molecules, the LSPR peak is blue-shifted as the size of the capping ligand increases. (2) When the ligands are macromolecular proteins, the LSPR property is similar to that of the overgrown nanoparticle (Au@gap@GNR) without thiolated biomolecules as capping agents. Interestingly, thiol-free and nonhomooligomeric DNA strands as capping agents present a similar influence in shaping the overgrowth of GNRs by varying their concentrations and sizes. In addition, the size effect of a DNA nanostructure was used to construct a ΔλLSPR-based catalytic nucleic acid biosensor using a DNA dendritic nanostructure as a capping agent combined with LSPR signals generated from the Au@gap@GNRs with morphological evolution. More importantly, the ΔλLSPR-based biosensor possesses three advantages in nucleic acid biosensing: (1) It is completely label- and wash-free, (2) it has an ultrahigh sensitivity and signal-to-noise ratio, and (3) it can be visualized without any instrumental aid, indicating a significant potential for ultrasensitive biosensing.

A highly sensitive platform is developed for the determination of microRNA-21 (miRNA-21) with inductively coupled plasma mass spectrometry (ICPMS). It includes the following operations: Hairpin structures DNA H1 and H2 are designed, and DNA H1 is bound to ultrasmall lanthanide upconversion nanoparticles (UCNPs) to produce UCNPs@DNA conjugate probes. Target miRNA triggers a chain reaction for alternating hybridization between DNA H1 (bound on UCNPs@DNA probe) and DNA H2. This leads to UCNPs accumulation and serves as an efficient amplification strategy for UCNPs. The concentration of miRNA-21 is closely correlated to the number of UCNPs; thus, the detection of 89Y by ICPMS provides a promising approach for miRNA quantification. This protocol exhibits high sensitivity to miRNA-21 within 0.1-500 fM, along with a detection limit of 41 aM, which is among the hitherto reported most sensitive procedures. It is worth mentioning that rare earth elements are scarcely present in living systems, which minimizes the background for ICPMS detection and excludes potential interferences from the coexisting species, which is most suited for biological assay.

Longitudinal surface plasmon resonance (LSPR)-based optical signals possess unique advantages in biomolecular sensing and detection which can be attributed to their ultrahigh sensitivity and signal-to-noise ratio. However, the lack of effective strategies for morphological control of gold nanorods (GNRs) complicates the precise tuning of their LSPR property. Herein, a "peptide-encoded" strategy was first developed to precisely control the morphologies of GNRs via overgrowth of GNR seeds in the presence of thiol-containing peptides. Significantly, the "peptide-encoded" GNRs exhibit a tunable LSPR peak ranging from 685 to 877 nm by altering the amount of peptide. A few obvious colorimetric changes were accompanied from pink to purple and even to blue. Other parameters, e.g., pH, temperature, and Ag+ concentration, could also be utilized to regulate the morphologies of the "peptide-encoded" GNRs. The ultrasensitive detection of tumor-related protease activities based on LSPR peak shifts was further successfully performed without the need for labeling or instrumental aid, achieving a limit of detection of 60 fM. It is much lower than traditional absorption-based analysis (1 nM) and enzyme-linked immunosorbent assay (ELISA) method (1 pM), indicating the great potential of this peptide-encoded strategy in the application of ultrasensitive biomarker assay and clinical diagnosis.

Microplasma optical-emission spectrometry (OES) is a promising technique for developing portable analytical instrumentations for real-time and on-site measurement of trace elemental species. However, its analytical performance is far from satisfactory for multielement analysis. Herein, a miniature OES system is developed for simultaneous multielement analysis with alternating-current-driven microplasma generated on the nozzle of a pneumatic micronebulizer as the excitation source. Because of the strong excitation capability of the microplasma and its sufficient contact with solution, a series of elements, including Ca, Cd, Co, Cr, Cu, Fe, K, Li, Mg, Mn, Na, Ni, Pb, and Zn, is directly excited in the spray with solution nebulization at a flow rate of 8 μL s–1. The characteristic optical emissions are measured by a charge-coupled-device (CCD) spectrometer. In addition, hydride generation is compatible with the present system, which makes it feasible for the simultaneous excitation of hydrides of As, Ge, Hg,...

Design and fabrication of smart liquid quantum dots (LQDs) with high biomolecule selectivity and specificity remains a challenge. Herein, a multifunctional calix[4]arene derivative (PCAD) was rationally designed and applied to fabricate a Tyr-responsive CdSe-LQD system through host-guest chemistry. Such a biosensor displays an outstanding fluorescence/macroscopic response for Tyr and reversible fluidic features due to the hydrogen interaction between the PCAD of CdSe-LQDs and Tyr. These excellent results highlighted CdSe-LQDs as a promising platform for biological molecule recognition and separation in the future.

Rapid detection of ultratrace pollutants in complex matrixes is a great challenge for studying their environmental behaviors and impacts. In this work, a method is developed by combining covalent organic framework (COF) based solid phase microextraction (SPME) with constant flow desorption ionization mass spectrometry for rapid detection of trace tetrabromobisphenol A (TBBPA) in multiple water media. The limits of detection and qualification are 0.92 and 3.1 ng L–1 for TBBPA, respectively. The linear range is between 0.01 and 10 μg L–1 (R2 = 0.9992), and the relative standard deviations with single fiber and multiple fibers are 6.4% and 6.7% (0.1 μg L–1, n = 9), respectively. The detection of nanogram per liter levels of TBBPA in tap water, river water, seawater, and beverage can be achieved in 7 min.

In single-cell analysis with ICP-MS it is highly important to ensure precise single-cell sampling into ICP. For this purpose, a simple configured pressure-resistant MicroCross interface is developed for high-throughput/high-precision microdroplet generation and single-cell encapsulation. Aqueous cell suspension is ejected and sheared into droplets by tangent-flowing hexanol-continuous phases in the flow-focusing geometry of MicroCross, wherein to precisely trap a single cell into a droplet, with an extremely low probability of

Fluorescent nanoparticles are widely used for sensing biologically significant species. However, there are only rare reports of the discrimination or speciation of metal species. In this work, we report for the first time the speciation of mercury (Hg2+) and methylmercury (CH3Hg+) by taking advantage of the fluorescence feature of folic-acid-capped gold nanoclusters (FA-AuNCs). FA-Au NCs exhibit an average size of 2.08 ± 0.15 nm and a maximum emission at λex/λem = 280/440 nm with a quantum yield of 27.3%. It is interesting that Hg2+ causes a significant quench of the fluorescence of FA-Au NCs, whereas CH3Hg+ leads to a remarkable fluorescence enhancement. On the basis of this discriminative fluorescent response between Hg2+ and CH3Hg+, a novel nanosensor for the speciation of CH3Hg+ and Hg2+ was developed, providing limits of detection (LODs) of 28 nM for Hg2+ and 25 nM for CH3Hg+ within 100–1000 nM. This sensing system is highly selective to mercury. Its practical applications were further demonstrated b...

A synthetic DNA machine performs quasi-mechanical movements in response to external intervention, suggesting the promise of constructing sensitive and specific biosensors. Herein, a smart DNA walker biosensor for label-free detection of carcinoembryonic antigen (CEA) is developed for the first time by a novel cascade amplification strategy of exonuclease (Exo) III-assisted target recycling amplification (ERA) and DNA walker. ERA as the first stage of amplification generates the walker DNA, while the autonomous traveling of the walker DNA on the substrate-modified silica microspheres as the second stage of amplification produces an ultrasensitive fluorescent signal with the help of N-methylmesoporphyrin IX (NMM). The DNA machine as a biosensor could be applied for transducing and quantifying signals from isothermal molecular amplifications, avoiding the complicated reporter elements and thermal cycling. The present biosensor achieves a detection limit of 1.2 pg·mL–1 within a linear range of 10 pg·mL–1 to 1...

The low atomization and excitation capability of nonthermal microplasma, e.g., dielectric barrier discharge (DBD), has greatly hampered its potential applications for the determination of metals in solution. In the present work, an inspiring development is reported for direct atomization and excitation of cadmium in aqueous solution by DBD and facilitates highly sensitive determination. A DBD microplasma is generated on the nozzle of a pneumatic micronebulizer to focus the DBD energy on a confined space and atomize/excite metals in the spray. Meanwhile, an appropriate sample matrix and nebulization in helium further improves the atomization and excitation capability of DBD. With cadmium as a model, its emission is recorded by a CCD spectrometer at 228.8 nm. By using an 80 μL sample solution nebulized at 3 μL s(-1), a linear range of 5-1000 μg L(-1) along with a detection limit of 1.5 μg L(-1) is achieved, which is comparable to those obtained by commercial bulky inductively coupled plasma (ICP)-based instrumentations.

The scope of dielectric barrier discharge (DBD) microplasma as a radiation source for optical emission spectrometry (OES) is extended by nickel carbonyl vapor generation. We proved that metal carbonyl completely avoids the extinguishing of plasma, and it is much more suitable for matching the DBD excitation and OES detection with respect to significant DBD quenching by concomitant hydrogen when hydride generation is used. A concentric quartz UV reactor allows sample solution to flow through the central channel wherein to efficiently receive the uniformly distributed UV irradiation in the confined cylindrical space between the concentric tubes, which facilitates effective carbonyl generation in a nickel solution. The carbonyl is transferred into the DBD excitation chamber by an argon stream for nickel excitation, and the characteristic emission of nickel at 232.0 nm is detected by a charge-coupled device (CCD) spectrometer. A 1.0 mL sample solution results in a linear range of 5-100 μg L(-1) along with a detection limit of 1.3 μg L(-1) and a precision of 2.4% RSD at 50 μg L(-1). The present DBD-OES system is validated by nickel in certified reference materials.

We report a new strategy for single supersaturated droplet analysis, i.e., the complicated hygroscopic properties of MgSO4 aerosols under supersaturated state were studied through the micro-Raman observation on an individual MgSO4 droplet deposited on a quartz substrate in a relative-humidity-controlled chamber. Upon reduction of the ambient relative humidity (RH), MgSO4 droplets with tiny volume lost water but did not effloresce. Thus, a detailed spectral evolution of the symmetric stretching vibration band (v1-SO4(2-)) from free ions (at approximately 983 cm(-1)) to monodentate (approximately 995 cm(-1)) and then to bidentate contact ion pairs (CIPs) or more complex chain-structural compositions (approximately 1021 cm(-1)) was observed with the high signal-to-noise (S/N) confocal Raman spectra of the droplet with a diameter of approximately 80 microns. Such a transition process could be well-described by the changes of relative intensity at 983, 995, and 1021 cm(-1). Four steps, i.e., concentrated step, monodentate CIPs step, bidentate CIPs step, and gel step, were roughly observed in the dehumidifying-humidifying cycle according to the intensity ratios of I995/I983 and I1021/I983. Even though the area ratio of the O-H stretching band of water molecules to the v1-SO4(2-) band seemed reversible in the dehumidifying and humidifying processes, the intensity ratios of I995/I983 and I1021/I983 showed a hysteresis in the decomposition of CIPs in the humidifying process with the RH40%. The O-H stretching envelope of the MgSO4 droplet was also observed to be sensitive to the structural changes of the hydrogen bonding of water molecules in the four steps. The intensity ratio of Raman scattering for the components with strong hydrogen bonds to those with weak ones, i.e., I3224/I3431, was used to understand the effects of CIPs on the water structures of the first hydration layer of Mg2+. Good consistency on the hysteresis in the humidifying process was also observed from the ratio of I3224/I3431 changing with RH.