Showing papers in "Analytical Chemistry in 2008"

Simple telemedicine for developing regions: camera phones and paper-based microfluidic devices for real-time, off-site diagnosis.

Abstract: This article describes a prototype system for quantifying bioassays and for exchanging the results of the assays digitally with physicians located off-site. The system uses paper-based microfluidic devices for running multiple assays simultaneously, camera phones or portable scanners for digitizing the intensity of color associated with each colorimetric assay, and established communications infrastructure for transferring the digital information from the assay site to an off-site laboratory for analysis by a trained medical professional; the diagnosis then can be returned directly to the healthcare provider in the field. The microfluidic devices were fabricated in paper using photolithography and were functionalized with reagents for colorimetric assays. The results of the assays were quantified by comparing the intensities of the color developed in each assay with those of calibration curves. An example of this system quantified clinically relevant concentrations of glucose and protein in artificial uri...

Fe3O4 Magnetic Nanoparticles as Peroxidase Mimetics and Their Applications in H2O2 and Glucose Detection

Abstract: Artificial enzyme mimetics are a current research interest because natural enzymes bear some serious disadvantages, such as their catalytic activity can be easily inhibited and they can be digested by proteases A very recently study reported by Yan et al has proven that Fe3O4 magnetic nanoparticles (MNPs) exhibit an intrinsic enzyme mimetic activity similar to that found in natural peroxidases, though MNPs are usually thought to be biological and chemical inert (Gao, L Z; Zhuang, J; Nie, L; Zhang, J B; Zhang, Y; Gu, N; Wang, T H; Feng, J; Yang, D L; Perrett, S; Yan, X Y Nat Nanotechnol 2007, 2, 577−583) In the present work, we just make use of the novel properties of Fe3O4 MNPs as peroxidase mimetics reported by Yan et al to detect H2O2 The Fe3O4 MNPs were prepared via a coprecipitation method The as-prepared Fe3O4 MNPs were then used to catalyze the oxidation of a peroxidase substrate 2,2‘-azino-bis(3-ethylbenzo-thiazoline-6-sulfonic acid) diammonium salt (ABTS) by H2O2 to the oxi

Visualization of GC/TOF-MS-based metabolomics data for identification of biochemically interesting compounds using OPLS class models.

Abstract: Metabolomics studies generate increasingly complex data tables, which are hard to summarize and visualize without appropriate tools The use of chemometrics tools, eg, principal component analysis (PCA), partial least-squares to latent structures (PLS), and orthogonal PLS (OPLS), is therefore of great importance as these include efficient, validated, and robust methods for modeling information-rich chemical and biological data Here the S-plot is proposed as a tool for visualization and interpretation of multivariate classification models, eg, OPLS discriminate analysis, having two or more classes The S-plot visualizes both the covariance and correlation between the metabolites and the modeled class designation Thereby the S-plot helps identifying statistically significant and potentially biochemically significant metabolites, based both on contributions to the model and their reliability An extension of the S-plot, the SUS-plot (shared and unique structure), is applied to compare the outcome of mu

Inkjet-printed microfluidic multianalyte chemical sensing paper

Abstract: This paper presents an inkjet printing method for the fabrication of entire microfluidic multianalyte chemical sensing devices made from paper suitable for quantitative analysis, requiring only a single printing apparatus. An inkjet printing device is used for the fabrication of three-dimensional hydrophilic microfluidic patterns (550-μm-wide flow channels) and sensing areas (1.5 mm × 1.5 mm squares) on filter paper, by inkjet etching, and thereby locally dissolving a hydrophobic poly(styrene) layer obtained by soaking of the filter paper in a 1 wt % solution of poly(styrene) in toluene. In a second step, the same inkjet printing device is used to print “chemical sensing inks”, comprising the necessary reagents for colorimetric analytical assays, into well-defined areas of the patterned microfluidic paper devices. The arrangement of the patterns, printed inks, and sensing areas was optimized to obtain homogeneous color responses. The results are “all-inkjet-printed” chemical sensing devices for the simult...

Laser ablation electrospray ionization (LAESI) for atmospheric pressure, in vivo, and imaging mass spectrometry

Abstract: The field of the invention is atmospheric pressure mass spectrometry (MS), and more specifically a process and apparatus which combine infrared laser ablation (LA) with electrospray ionization (ESI).

Low-temperature plasma probe for ambient desorption ionization.

Abstract: A low-temperature plasma (LTP) probe has been developed for ambient desorption ionization. An ac electric field is used to induce a dielectric barrier discharge through use of a specially designed electrode configuration. The low-temperature plasma is extracted from the probe where it interacts directly with the sample being analyzed, desorbing and ionizing surface molecules in the ambient environment. This allows experiments to be performed without damage to the sample or underlying substrate and, in the case of biological analysis on skin surfaces, without electrical shock or perceptible heating. Positive or negative ions are produced from a wide range of chemical compounds in the pure state and as mixtures in the gaseous, solution, or condensed phases, using He, Ar, N2, or ambient air as the discharge gas. Limited fragmentation occurs, although it is greater in the cases of the molecular than the atomic discharge gases. The effectiveness of the LTP probe has been demonstrated by recording characteristi...

Paper-based microfluidic devices by plasma treatment.

Abstract: Paper-based microfluidic patterns have been demonstrated in recent literature to have a significant potential in developing low-cost analytical devices for telemedicine and general health monitoring. This study reports a new method for making microfluidic patterns on a paper surface using plasma treatment. Paper was first hydrophobized and then treated using plasma in conjunction with a mask. This formed well defined hydrophilic channels on the paper. Paper-based microfluidic systems produced in this way retained the flexibility of paper and a variety of patterns could be formed. A major advantage of this system is that simple functional elements such as switches and filters can be built into the patterns. Examples of these elements are given in this study.

Gold nanoparticle-based colorimetric assay for the direct detection of cancerous cells.

Abstract: Early and accurate detection of cancer often requires time-consuming techniques and expensive instrumentation. To address these limitations, we developed a colorimetric assay for the direct detection of diseased cells. The assay uses aptamer-conjugated gold nanoparticles to combine the selectivity and affinity of aptamers and the spectroscopic advantages of gold nanoparticles to allow for the sensitive detection of cancer cells. Samples with the target cells present exhibited a distinct color change while nontarget samples did not elicit any change in color. The assay also showed excellent sensitivity with both the naked eye and based on absorbance measurements. In addition, the assay was able to differentiate between different types of target and control cells based on the aptamer used in the assay indicating the wide applicability of the assay for diseased cell detection. On the basis of these qualities, aptamer-conjugated gold nanoparticles could become a powerful tool for point of care diagnostics.

Low-cost printing of poly(dimethylsiloxane) barriers to define microchannels in paper.

Abstract: This paper describes the use of a modified x,y-plotter to generate hydrophilic channels by printing a solution of hydrophobic polymer (pol(dimethylsiloxane; PDMS) dissolved in hexanes onto filter paper. The PDMS penetrates the depth of the paper and forms a hydrophobic wall that aqueous solutions cannot cross. The minimum size of printed features is ∼1 mm; this resolution is adequate for the rapid prototyping of hand-held, visually read, diagnostic assays (and other microfluidic systems) based on paper. After curing the printed PDMS, the paper-based devices can be bent or folded to generate three-dimensional systems of channels. Capillary action pulls aqueous samples into the paper channels. Colorimetric assays for the presence of glucose and protein are demonstrated in the printed devices; spots of Bromothymol Blue distinguished samples with slightly basic pH (8.0) from samples with slightly acidic pH (6.5). The work also describes using printed devices that can be loaded using multipipets and printed fl...

Relative Quantification of Proteins in Human Cerebrospinal Fluids by MS/MS Using 6-Plex Isobaric Tags

Abstract: A new 6-plex isobaric mass tagging technology is presented, and proof of principle studies are carried out using standard protein mixtures and human cerebrospinal fluid (CSF) samples. The Tandem Mass Tags (TMT) comprise a set of structurally identical tags which label peptides on free amino-terminus and epsilon-amino functions of lysine residues. During MS/MS fragmentation, quantification information is obtained through the losses of the reporter ions. After evaluation of the relative quantification with the 6-plex version of the TMT on a model protein mixture at various concentrations, the quantification of proteins in CSF samples was performed using shotgun methods. Human postmortem (PM) CSF was taken as a model of massive brain injury and comparison was carried out with antemortem (AM) CSF. After immunoaffinity depletion, triplicates of AM and PM CSF pooled samples were reduced, alkylated, digested by trypsin, and labeled, respectively, with the six isobaric variants of the TMT (with reporter ions from...

Nonenzymatic Electrochemical Glucose Sensor Based on Nanoporous PtPb Networks

Abstract: Here, we report on a novel nonenzymatic amperometric glucose sensor based on three-dimensional PtPb networks directly grown on Ti substrates using a reproducible one-step hydrothermal method. The surface morphology and bimetallic composition of the synthesized nanoporous PtPb materials were characterized using scanning electron microscopy and energy-dispersive X-ray spectrometry, respectively. Voltammetry and amperometric methods were used to evaluate the electrocatalytic activities of the synthesized electrodes toward nonenzymatic glucose oxidation in neutral media in the absence and in the presence of chloride ions. The synthesized nanoporous PtPb electrodes have strong and sensitive current responses to glucose. Their amperometric sensitivities increase in the order of Pt-Pb (0%) < Pt-Pb (30%) < Pt-Pb (70%) < Pt-Pb (50%). These nanoporous PtPb electrodes are also highly resistant toward poisoning by chloride ions and capable of sensing glucose amperometrically at a very low potential, -80 mV (Ag/AgCl), where the interference from the oxidation of common interfering species such as ascorbic acid, acetamidophenol, and uric acid is effectively avoided.

Electrostatic repulsion hydrophilic interaction chromatography for isocratic separation of charged solutes and selective isolation of phosphopeptides.

Abstract: If an ion-exchange column is eluted with a predominantly organic mobile phase, then solutes can be retained through hydrophilic interaction even if they have the same charge as the stationary phase This combination is termed electrostatic repulsion-hydrophilic interaction chromatography (ERLIC) With mixtures of solutes that differ greatly in charge, repulsion effects can be exploited to selectively antagonize the retention of the solutes that normally would be the best retained This permits the isocratic resolution of mixtures that normally require gradients, including peptides, amino acids, and nucleotides ERLIC affords convenient separations of highly charged peptides that cannot readily be resolved by other means In addition, phosphopeptides can be isolated selectively from a tryptic digest

Gold Nanoparticle-Based Colorimetric and “Turn-On” Fluorescent Probe for Mercury(II) Ions in Aqueous Solution

Abstract: An approach for visual and fluorescent sensing of Hg2+ in aqueous solution is presented. This method is based on the Hg2+-induced conformational change of a thymine (T)-rich single-stranded DNA (ssDNA) and the difference in electrostatic affinity between ssDNA and double-stranded (dsDNA) with gold nanoparticles. The dye-tagged ssDNA containing T−T mismatched sequences was chosen as Hg2+ acceptor. At high ionic strength, introduction of the ssDNA to a colloidal solution of the aggregates of gold nanoparticles results in color change, from blue-gray to red of the solution, and the fluorescence quenching of the dye. Binding of Hg2+ with the ssDNA forms the double-stranded structure. This formation of dsDNA reduces the capability to stabilize bare nanoparticles against salt-induced aggregation, remaining a blue-gray in the color of the solution, but fluorescence signal enhancement compared with that without Hg2+. With the optimum conditions described, the system exhibits a dynamic response range for Hg2+ from...

Fundamentals of Traveling Wave Ion Mobility Spectrometry

Abstract: Traveling wave ion mobility spectrometry (TW IMS) is a new IMS method implemented in the Synapt IMS/mass spectrometry system (Waters). Despite its wide adoption, the foundations of TW IMS were only qualitatively understood and factors governing the ion transit time (the separation parameter) and resolution remained murky. Here we develop the theory of TW IMS using derivations and ion dynamics simulations. The key parameter is the ratio (c) of ion drift velocity at the steepest wave slope to wave speed. At low c, the ion transit velocity is proportional to the squares of mobility (K) and electric field intensity (E), as opposed to linear scaling in drift tube (DT) IMS and differential mobility analyzers. At higher c, the scaling deviates from quadratic in a way controlled by the waveform profile, becoming more gradual with the ideal triangular profile but first steeper and then more gradual for realistic profiles with variable E. At highest c, the transit velocity asymptotically approaches the wave speed. ...

High-Precision Laser Spectroscopy D/H and 18O/16O Measurements of Microliter Natural Water Samples

Abstract: Newly available gas analyzers based on off-axis integrated cavity output spectroscopy (OA-ICOS) lasers have been advocated as an alternative to conventional isotope-ratio mass spectrometers (IRMS) for the stable isotopic analysis of water samples In the case of H2O, OA-ICOS is attractive because it has comparatively low capital and maintenance costs, the instrument is small and field laboratory portable, and provides simultaneous D/H and 16O/18O ratio measurements directly on H2O molecules with no conversion of H2O to H2, CO, or H2/CO2−water equilibration required Here we present a detailed assessment of the performance of a liquid-water isotope analyzer, including instrument precision, estimates of sample memory and sample mass effects, and instrumental drift We provide a recommended analysis procedure to achieve optimum results using OA-ICOS Our results show that, by using a systematic sample analysis and data normalization procedure routine, measurement accuracies of ± 08‰ for δD and ±01‰ δ18O ar

Micro total analysis systems: latest achievements.

Abstract: Technology 4403 Microfabrication 4403 Assembly and Interfacing 4404 Optical Integration 4405 Flow Control 4405 Standard Operations 4406 Sample Preparation 4406 Injection and Separation 4407 Fluidic Reactors 4407 Particle and Cell Sorting 4409 Cell Trapping and Culture 4409 Applications 4410 Clinical Diagnostics 4410 Nucleic Acids 4411 Proteins 4412 Cell and Tissue Studies 4413 Environmental Monitoring 4414 Literature Cited 4414

High-throughput quantitative polymerase chain reaction in picoliter droplets.

Abstract: Limiting dilution PCR has become an increasingly useful technique for the detection and quantification of rare species in a population, but the limit of detection and accuracy of quantification are largely determined by the number of reactions that can be analyzed. Increased throughput may be achieved by reducing the reaction volume and increasing processivity. We have designed a high-throughput microfluidic chip that encapsulates PCR reagents in millions of picoliter droplets in a continuous oil flow. The oil stream conducts the droplets through alternating denaturation and annealing zones, resulting in rapid (55-s cycles) and efficient PCR amplification. Inclusion of fluorescent probes in the PCR reaction mix permits the amplification process to be monitored within individual droplets at specific locations within the microfluidic chip. We show that amplification of a 245-bp adenovirus product can be detected and quantified in 35 min at starting template concentrations as low as 1 template molecule/167 droplets (0.003 pg/microL). The frequencies of positive reactions over a range of template concentrations agree closely with the frequencies predicted by Poisson statistics, demonstrating both the accuracy and sensitivity of this platform for limiting dilution and digital PCR applications.

Nanomolar and selective determination of epinephrine in the presence of norepinephrine using carbon paste electrode modified with carbon nanotubes and novel 2-(4-oxo-3-phenyl-3,4-dihydro-quinazolinyl)-N'-phenyl-hydrazinecarbothioamide.

Abstract: A novel modified carbon nanotube paste electrode of 2-(4-oxo-3-phenyl-3,4-dihydro-quinazolinyl)-N′-phenyl-hydrazinecarbothioamide (2PHC) was fabricated, and the electro-oxidation of epinephrine (EP), norepinephrine (NE), and their mixture has been studied using electrochemical methods. The modified electrode displayed strong catalytic function for the oxidation of EP and NE and resolved the overlap voltammetric response of EP and NE into two well-defined voltammetric peaks of about 240 mV with square wave voltammetry (SWV). A linear response in the range of (5 × 10−8)−(5.5 × 10−4) M with a detection limit (S/N = 3) of 9.4 nM for EP was obtained.

Equilibrium separation and filtration of particles using differential inertial focusing.

Abstract: Rapid separation and filtration of particles in solution has a wide range of applications including blood cell separation, ultrasound contrast agent preparation, and purification of fermentation products. However, current techniques that provide quick processing rates are high in complexity. We present a rapid microfluidic filtration technology capable of separating particles based on size, with purities from 90 to 100% and high-volume throughputs of 1 mL/min. Data for separation of rigid particles, deformable emulsions, and platelets from whole blood are presented. The system is based upon differential inertial focusing of particles of varying sizes and allows continuous separation based only on intrinsic hydrodynamic forces developed in a flow through an asymmetrically curved channel. A theoretical description of the underlying forces is developed, and in combination with data determining a size cutoff for separation, a semiempirical relationship describing how channel geometry is related to this cutoff is shown. Cascading separations in series is shown to be useful for increasing purity and yield. This type of microfluidic system can filter deformable particles, is largely independent of particle density, and can provide throughputs typical of macroscale filtration in a compact format, enabling applications in blood filtration and particle concentration.

Ultralow Fouling and Functionalizable Surface Chemistry Based on a Zwitterionic Polymer Enabling Sensitive and Specific Protein Detection in Undiluted Blood Plasma

Abstract: A crucial step in the development of implanted medical devices, in vivo diagnostics, and microarrays is the effective prevention of nonspecific protein adsorption from real-world complex media such as blood plasma or serum. In this work, a zwitterionic poly(carboxybetaine acrylamide) (polyCBAA) biomimetic material was employed to create a unique biorecognition coating with an ultralow fouling background, enabling the sensitive and specific detection of proteins in blood plasma. Conditions for surface activation, protein immobilization, and surface deactivation of the carboxylate groups in the polyCBAA coating were determined. An antibody-functionalized polyCBAA surface platform was used to detect a target protein in blood plasma using a sensitive surface plasmon resonance (SPR) sensor. A selective protein was directly detected from 100% human blood plasma with extraordinary specificity and sensitivity. The total nonspecific protein adsorption on the functionalized polyCBAA surface was very low (<3 ng/cm2 ...

Natural organic matter and the event horizon of mass spectrometry.

Abstract: Soils, sediments, freshwaters, and marine waters contain natural organic matter (NOM), an exceedingly complex mixture of organic compounds that collectively exhibit a nearly continuous range of pro...

Toward a generic extraction method for simultaneous determination of pesticides, mycotoxins, plant toxins, and veterinary drugs in feed and food matrixes.

Abstract: A fast and straightforward generic procedure for the simultaneous extraction of various classes of pesticides, mycotoxins, plant toxins, and veterinary drugs in various matrixes has been developed, for subsequent analysis by liquid chromatography with mass spectrometric detection. As a first step, four existing multianalyte procedures and three newly proposed methods were compared for a test set of 172 pesticides, mycotoxins, and plant toxins spiked to a feed matrix. The new procedures, which basically involved extraction/dilution of the sample with water and an acidified organic solvent (methanol, acetonitrile, or acetone), were most promising. The three new generic extraction methods were further tested for applicability to other matrixes (maize, honey, milk, egg, meat). Overall, the best recoveries were obtained for acetone, followed by acetonitrile. With respect to matrix effects, acetonitrile was the most favorable solvent and methanol was the worst. The occurrence of matrix effects decreased for the...

Ultrasensitive electrochemical immunosensor for clinical immunoassay using thionine-doped magnetic gold nanospheres as labels and horseradish peroxidase as enhancer.

Abstract: A new signal amplification strategy based on thionine (TH)-doped magnetic gold nanospheres as labels and horseradish peroxidase (HRP) as enhancer holds promise to improve the sensitivity and detection limit of the immunoassay for carcinoembryonic antigen (CEA), as a model protein. This immunoassay system was fabricated on a carbon fiber microelectrode (CFME) covered with a well-ordered anti-CEA/protein A/nanogold architecture. The reverse micelle method was initially used for the preparation of TH-doped magnetic gold nanospheres (nanospheres), and the synthesized nanospheres were then labeled on HRP-bound anti-CEA as a secondary antibody (bionanospheres). Sandwich-type protocol was successfully introduced to develop a new high-efficiency electrochemical immunoassay with the labeled bionanospheres toward the reduction of H2O2. Under optimized conditions, the linear range of the proposed immunoassay without HRP as enhancer was 1.2−125 ng/mL CEA, whereas the assay sensitivity by using HRP as enhancer could b...

Nanofluidic devices and their applications.

Abstract: Recent developments in micro- and nanotechnologies made possible the fabrication of devices integrating a deterministic network of nanochannels, i.e., with at least one dimension in a range from 1 to 100 nm. The proximity of this dimension and the Debye length, the size of biomolecules such as DNA or proteins, or even the slip length, added to the excellent control on the geometry gives unique features to nanofluidic devices. This new class of devices not only finds applications wherever less well-defined porous media, such as electrophoresis gels, have been traditionally used but also give a new insight into the sieving mechanisms of biomolecules and the fluid flow at the nanoscale. Beyond this, the control on the geometry allows smarter design resulting, among others, in new separation principles by taking advantage of the anisotropy. This perspective gives an overview on the fabrication technologies of nanofluidic devices and their applications. In the first part, the current state of the art of nanofl...

Ion-Selective Electrodes Using Carbon Nanotubes as Ion-to-Electron Transducers

Abstract: This study developed a new type of all-solid-state ion-selective electrode based on a transducing layer of a network of single-walled carbon nanotubes. The extraordinary capacity of carbon nanotubes to promote electron transfer between heterogeneous phases made the presence of electroactive polymers or any other ion-to-electron-transfer promoter unnecessary. The new transducer layer was characterized by environmental scanning electron microscopy and electrochemical impedance spectroscopy. The stability of the electrical potential of the new solid-contact electrode was examined by performing current-reversal chronopotentiometry, and the influence of the interfacial water film was assessed by the potentiometric water layer test. The performance of the new electrode was evaluated by determining K+ with an ion-selective membrane that contained the well-known valinomycin ion carrier. The new electrode had a Nernstian slope (58.4 mV/decade), dynamic ranges of four logarithmic units, and selectivities and limits...

Amine-capped ZnS-Mn2+ nanocrystals for fluorescence detection of trace TNT explosive.

Abstract: Mn2+-doped ZnS nanocrystals with an amine-capping layer have been synthesized and used for the fluorescence detection of ultratrace 2,4,6-trinitrotoluene (TNT) by quenching the strong orange Mn2+ photoluminescence. The organic amine-capped nanocrystals can bind TNT species from solution and atmosphere by the acid−base pairing interaction between electron-rich amino ligands and electron-deficient aromatic rings. The resultant TNT anions bound onto the amino monolayer can efficiently quench the Mn2+ photoluminescence through the electron transfer from the conductive band of ZnS to the lowest unoccupied molecular orbital (LUMO) of TNT anions. The amino ligands provide an amplified response to the binding events of nitroaromatic compounds by the 2- to ∼5-fold increase in quenching constants. Moreover, a large difference in quenching efficiency was observed for different types of nitroaromatic analytes, dependent on the affinity of nitro analytes to the amino monolayer and their electron-accepting abilities. T...

High-speed and high-resolution UPLC separation at zero degrees Celsius.

Abstract: The conformational properties of proteins can be probed with hydrogen/deuterium exchange mass spectrometry (HXMS). In order to maintain the deuterium label during LC/MS analyses, chromatographic separation must be done rapidly (usually in under 8−10 min) and at 0 °C. Traditional RP-HPLC with ∼3-μm particles has shown generally poor chromatographic performance under these conditions and thereby has been prohibitive for HXMS analyses of larger proteins and many protein complexes. Ultraperformance liquid chromatography (UPLC) employs particles smaller than 2 μm in diameter to achieve superior resolution, speed, and sensitivity as compared to HPLC. UPLC has previously been shown to be compatible with the fast separation and low temperature requirements of HXMS. Here we present construction and validation of a custom UPLC system for HXMS. The system is based on the Waters nanoACQUITY platform and contains a Peltier-cooled module that houses the injection and switching valves, online pepsin digestion column, an...

MALDI-FTICR Imaging Mass Spectrometry of Drugs and Metabolites in Tissue

Abstract: A new approach is described for imaging mass spectrometry analysis of drugs and metabolites in tissue using matrix-assisted laser desorption ionization-Fourier transform ion cyclotron resonance (MALDI-FTICR). The technique utilizes the high resolving power to produce images from thousands of ions measured during a single mass spectrometry (MS)-mode experiment. Accurate mass measurement provides molecular specificity for the ion images on the basis of elemental composition. Final structural confirmation of the targeted compound is made from accurate mass fragment ions generated in an external quadrupole-collision cell. The ability to image many small molecules in a single measurement with high specificity is a significant improvement over existing MS/MS based technologies. Example images are shown for olanzapine in kidney and liver and imatinib in glioma.

In Vivo Study of Biodistribution and Urinary Excretion of Surface-Modified Silica Nanoparticles

Abstract: The biodistribution and urinary excretion of different surface-modified silica nanoparticles (SiNPs) in mice were investigated in situ using an in vivo optical imaging system. Three types of surface-modified SiNPs, including OH-SiNPs, COOH-SiNPs, and PEG-SiNPs with a size of ∼45 nm, have been prepared with RuBPY doped for imaging purposes. Intravenous (iv) injection of these SiNPs followed by fluorescence tracing in vivo using the Maestro in vivo imaging system indicated that OH-SiNPs, COOH-SiNPs, and PEG-SiNPs were all cleared from the systemic blood circulation, but that both the clearance time and subsequent biological organ deposition were dependent on the surface chemical modification of the SiNPs. Thus, for instance, the PEG-SiNPs exhibited relatively longer blood circulation times and lower uptake by the reticuloendothelial system organs than OH-SiNPs and COOH-SiNPs. More interestingly, in vivo real-time imaged dominant signal in bladder and urine excretion studies revealed that all three types of ...

Gold Nanoelectrode Ensembles for the Simultaneous Electrochemical Detection of Ultratrace Arsenic, Mercury, and Copper

Abstract: Simultaneous electrochemical detection of As(III), Hg(II), and Cu(II) using a highly sensitive platform based on gold nanoelectrode ensembles (GNEEs) is described. GNEEs were grown by colloidal chemical approach on thiol-functionalized sol—gel derived three-dimensional silicate network preassembled on a polycrystalline gold (Au) electrode. GNEEs on the silicate network have been characterized by field emission scanning electron microscopy, X-ray diffraction, diffuse reflectance spectroscopy, and electrochemical measurements. Square wave anodic stripping voltammetry (SWASV) has been used for the detection of As(III) and Hg(II) without any interference from Cu(II) at the potentials of 0.06 and 0.53 V, respectively. The GNEE electrode is highly sensitive, and it shows linear response for As(III) and Hg(II) up to 15 ppb. The detection limit (signal-to-noise ratio = 4) of the GNEE electrode toward As(III) and Hg(II) is 0.02 ppb, which is well below the guideline value given by the World Health Organization (WH...