In recent years, microplastics have been found in seawater, soil, food, and even human blood and tissues. The ubiquity of microplastics is alarming, but the health and environmental impacts of microplastics are just beginning to be understood. Accordingly, sampling, separating, and quantifying exposure to microplastics to devise a total risk assessment is the focus of ongoing research.
View Article and Find Full Text PDFWe report a systematic study of the electrocatalytic properties and stability of a series of 1-2 nm Au, Pd, and AuPd alloy nanoparticles (NPs) for the ethanol oxidation reaction (EOR). Following EOR electrocatalysis, NP sizes and compositions were characterized using aberration-corrected scanning transmission electron microscopy (ac-STEM) and energy dispersive spectroscopy (EDS). Two main findings emerge from this study.
View Article and Find Full Text PDFA key goal of nanoparticle-based catalysis research is to correlate the structure of nanoparticles (NPs) to their catalytic function. The most common approach for achieving this goal is to synthesize ensembles of NPs, characterize the ensemble, and then evaluate its catalytic properties. This approach is effective, but it excludes the certainty of structural heterogeneity in the NP ensemble.
View Article and Find Full Text PDFWe report on the use of silver nanodisks (AgNDs), having a diameter of 50 ± 8 nm and a thickness of 8 ± 2 nm, as electrochemical labels for the detection of a model metalloimmunoassay for the heart failure biomarker NT-proBNP. The detection method is based on an electrochemically activated galvanic exchange (GE) followed by the detection of Ag using anodic stripping voltammetry (ASV). The AgNDs labels are superior to Ag nanocubes and Ag nanospheres in terms of the dynamic range for both the model and NT-proBNP metalloimmunoassays.
View Article and Find Full Text PDFWe report the presence of small clusters of atoms (<1 nm) (SCs) and single atoms (SAs) in solutions containing 1-2 nm dendrimer-encapsulated nanoparticles (DENs). Au and Pd DENs were imaged using aberration-corrected scanning transmission electron microscopy (ac-STEM), and energy dispersive spectroscopy (EDS) was used to identify and quantify the SAs/SCs. Two main findings have emerged from this work.
View Article and Find Full Text PDFHere we report an easily fabricated, plastic-based lateral flow device for carrying out metalloimmunoassays. The device is called Flow to emphasize the open-channel design. We have shown that the Flow is capable of magnetic microbead (MμB)-based metalloimmunoassays for the detection of two types of immunoconjugates: a model composite (MC) and a sandwich immunoassay for the heart failure marker NT-proBNP.
View Article and Find Full Text PDFIn this article, we compare linear sweep anodic stripping voltammetry (LASV) and square-wave anodic stripping voltammetry (SWASV) for detection of a nano metalloimmunoassay. Two separate immunoassays were examined: a model assay, based on interactions between antibodies, and a sandwich assay for the heart failure marker NT-proBNP. In both cases, one antibody is linked to a magnetic microbead, and one is linked to a spherical Ag nanoparticle label.
View Article and Find Full Text PDFThe concept of nanoparticle-mediated electron transfer (eT) across insulating thin films was elucidated theoretically by Allongue and Chazalviel in 2011. In their model, metal nanoparticles (NPs) are immobilized atop passivating, self-assembled monolayers (SAMs). They found that under certain conditions, related to the thickness of the SAM and the size of the NPs, efficient faradaic oxidation and reduction reactions could proceed at the NP surface.
View Article and Find Full Text PDFWe report a method for electrochemical pH regulation in microdroplets generated in a microfluidic device. The key finding is that controlled quantities of reagents can be generated electrochemically in moving microdroplets confined within a microfluidic channel. Additionally, products generated at the anode and cathode can be isolated within descendant microdroplets.
View Article and Find Full Text PDFHere we use experiments and finite element simulations to investigate the electrokinetics within straight microchannels that contain a bipolar electrode and an unbuffered electrolyte solution. Our findings indicate that in the presence of a sufficiently high electric field, water electrolysis proceeds at the bipolar electrode and leads to variations in both solution conductivity and ionic current density along the length of the microchannel. The significance of this finding is twofold.
View Article and Find Full Text PDFWe report a method for synthesizing and studying shape-controlled, single Pt nanoparticles (NPs) supported on carbon nanoelectrodes. The key advance is that the synthetic method makes it possible to produce single, electrochemically active NPs with a vast range of crystal structures and sizes. Equally important, the NPs can be fully characterized, and, therefore, the electrochemical properties of the NPs can be directly correlated to the size and structure of a single shape.
View Article and Find Full Text PDFACS Appl Nano Mater
October 2021
In this paper we demonstrate the use of dual-shaped silver nanoparticles (AgNPs) as detection labels for electrochemical bioassays. The key finding is that by using AgNP labels having two different shapes simultaneously, the limit of detection (LOD) for the assays is lowered compared to using either of the two shapes separately. The two shapes were silver nanocubes (AgNCs) having edge lengths of 40 ± 4 nm and spherical AgNPs (sAgNPs) having diameters of 20 ± 3 nm.
View Article and Find Full Text PDFThe effect of serum on electrochemical detection of bioassays having silver nanoparticle (AgNP) detection labels was investigated. Both a model assay and an antigen-specific sandwich bioassay for the heart failure marker NT-proBNP were examined. In both cases, the AgNP labels were conjugated to a detection antibody.
View Article and Find Full Text PDFHere, we report on the use of 40 ± 4 nm silver nanocubes (AgNCs) as electrochemical labels in bioassays. The model metalloimmunoassay combines galvanic exchange (GE) and anodic stripping voltammetry (ASV). The results show that a lower limit of detection is achieved by simply changing the shape of the Ag label yielding improved GE with AgNCs when compared to GE with spherical silver nanoparticles (sAgNPs).
View Article and Find Full Text PDFPeptide-functionalized nanoparticles (NPs) often rely on a well-defined peptide structure to function. Here, we report the attachment of model peptides to the ligand shell of AuNPs passivated with oligoethylene glycol (OEG). Specifically, peptides containing the repeating (LLKK) motif plus either one or two reactive functional groups were covalently linked to OEG-capped, ∼5 nm AuNPs via the Cu-catalyzed azide-alkyne cycloaddition reaction.
View Article and Find Full Text PDFIn this article, we report continuous sorting of two microplastics in a trifurcated microfluidic channel using a new method called serial faradaic ion concentration polarization (fICP). fICP is an electrochemical method for forming ion depletion zones and their corresponding locally elevated electric fields in microchannels. By tuning the interplay between the forces of electromigration and convection during a fICP experiment, it is possible to control the flow of charged objects in microfluidic channels.
View Article and Find Full Text PDFHere we report on hydride-terminated (HT) electrodeposition of Pt multilayers onto ∼1.6 nm Au nanoparticles (NPs). The results build on our earlier findings regarding electrodeposition of a single monolayer of Pt onto Au NPs and reports relating to HT Pt electrodeposition onto bulk Au.
View Article and Find Full Text PDFPathogenic variants within PAX6 are most often associated with aniridia, but have been linked with other phenotypes such as nystagmus, cataracts and foveal hypoplasia. Data are presented from a large cohort of 434 probands referred for PAX6 diagnostic testing. This analysis identified a wide range of pathogenic variants (n = 145) in 254 probands (including 61 novel variants).
View Article and Find Full Text PDFIn the present article we report a new hybrid microfluidic device (hyFlow) comprising a disposable paper electrode and a three-dimensional (3D) printed plastic chip for the electrochemical detection of a magnetic bead-silver nanoparticle (MB-AgNP) bioconjugate. This hybrid device evolved due to the difficulty of incorporating micron-scale MBs into paper-only fluidic devices. Specifically, paper fluidic devices can entrap MB-containing conjugates within their cellulose or nitrocellulose fiber matrix.
View Article and Find Full Text PDFIn this paper, we demonstrate an electrochemical method for detection of the heart failure biomarker, N-terminal prohormone brain natriuretic peptide (NT-proBNP). The approach is based on a paper electrode assembly and a metalloimmunoassay; it is intended for eventual integration into a home-use sensor. Sensing of NT-proBNP relies on the formation of a sandwich immunoassay and electrochemical quantification of silver nanoparticle (AgNP) labels attached to the detection antibodies (Abs).
View Article and Find Full Text PDFIn this article, experiment and theory are combined to analyze Pb and Cu underpotential deposition (UPD) on ∼1.7 nm Au nanoparticles (NPs) and the AuPt structures that result after galvanic exchange (GE) of the UPD layer for Pt. Experimental Pb (0.
View Article and Find Full Text PDFHere we report on the use of heterobifunctional cross-linkers (HBCLs) to control the number, orientation, and activity of immunoglobulin G antibodies (Abs) conjugated to silver nanoparticles (AgNPs). A hydrazone conjugation method resulted in exclusive modification of the polysaccharide chains present on the fragment crystallizable region of the Abs, leaving the antigen-binding regions accessible. Two HBCLs, each having a hydrazide terminal group, were synthesized and tested for effectiveness.
View Article and Find Full Text PDFThe relationship between experiment and theory in electrocatalysis is one of profound importance. Until fairly recently, the principal role of theory in this field was interpreting experimental results. Over the course of the past decade (roughly the period covered by this review), however, that has begun to change, with theory now frequently leading the design of electrocatalytic materials.
View Article and Find Full Text PDFWe are interested in functionalizing gold nanoparticles (AuNPs) with proteins using a biomimetic approach in which an intermediate peptide "glue" directs the orientation of a protein relative to the AuNP surface. The first step toward this goal is described in the present article. Specifically, we show that ∼5 nm AuNPs can be functionalized with a mixed self-assembled monolayer (SAM) consisting of oligo(ethylene glycol) alkanethiols terminated with either hydroxyl or azide groups, and that the resulting materials are stable and soluble in water.
View Article and Find Full Text PDFHere we report on the seemingly simple process of galvanic exchange (GE) between electrogenerated AuCl and silver nanoparticles (AgNPs). The results were obtained in the specific context of using AgNPs as labels for bioassays in paper fluidic devices. Results obtained from a combined electrochemistry and microscopy study indicate that the GE process results in recovery of only ∼5% of the total equivalents of Ag present in the system.
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