In observing the electrocatalytic current of nanoparticles (NPs) using single-entity electrochemistry (SEE), the surface state of the NPs significantly influences the SEE signal. This study investigates the influence of capping agents on the electrocatalytic properties of gold (Au) NPs using SEE. Two inner-sphere reactions, hydrazine oxidation and glucose oxidation, were chosen to explore the SEE characteristics of Au NPs based on the capping agent presence.
View Article and Find Full Text PDFSingle-entity electrochemistry (SEE) enables research into the electrochemical properties of nanoparticles (NPs) at the individual NP level. Recent studies on active particle-active electrode systems have expanded the scope of SEE measurements, moving beyond the limitations of inert electrode-based methods that rely on distinct NP-electrode catalytic differences, thereby enhancing mechanistic understanding of catalytic reactions. In this study, we investigated SEE signals from Pt NPs colliding with Au ultramicroelectrodes (UME) at elevated potentials where both Pt and Au UME exhibit electrocatalytic activity.
View Article and Find Full Text PDFFor the first time, single-entity electrochemistry (SEE) was demonstrated in a hydrogel matrix. SEE involves the investigation of the electrochemical characteristics of individual nanoparticles (NPs) by observing the signal generated when a single NP, suspended in an aqueous solution, collides with an electrode and triggers catalytic reactions. Challenges associated with SEE in electrolyte-containing solutions such as signal variation due to NP aggregation and noise fluctuation caused by convection phenomena can be addressed by employing a hydrogel matrix.
View Article and Find Full Text PDFThis work demonstrates the utilization of short-time Fourier transform (STFT), and continuous wavelet transform (CWT) electrochemical impedance spectroscopy (EIS) for time-resolved analysis of stochastic collision events of platinum nanoparticles (NPs) onto gold ultramicroelectrode (UME). The enhanced electrocatalytic activity is observed in both chronoamperometry (CA) and EIS. CA provides the impact moment and rough estimation of the size of NPs.
View Article and Find Full Text PDFNanomaterials (Basel)
April 2023
Nanomaterials have been instrumental in the development of electrochemical nano-biosensors, offering high sensitivity and selectivity [...
View Article and Find Full Text PDFCollision (or impact) of single palladium nanoparticles (Pd NPs) on gold (Au), copper (Cu), nickel (Ni), and platinum (Pt) ultramicroelectrodes (UMEs) were investigated via electrocatalytic amplification method. Unlike the blip responses of previous Pd NP collision studies, the staircase current response was obtained with the Au UME. The current response, including collision frequency and peak magnitude, was analyzed depending on the material of the UME and the applied potential.
View Article and Find Full Text PDFA single silver (Ag) nanoparticle (NP) collision was observed and analyzed in an alkaline solution using the electrocatalytic amplification (EA) method. Previously, the observation of a single Ag NP collision was only possible through limited methods based on a self-oxidation of Ag NPs or a blocking strategy. However, it is difficult to characterize the electrocatalytic activity of Ag NPs at a single NP level using a method based on the self-oxidation of Ag NPs.
View Article and Find Full Text PDFThe immunoglobulin E (IgE) level in serum is an important factor in the examination of allergy. Ferrocene (Fc)-modified self-assembled monolayers (SAMs) were placed on an indium tin oxide (ITO) electrode as a sensing layer for the detection of human IgE. The Fc moiety in the SAMs facilitated the electron transfer through the organic SAMs layer and electrocatalytic signal amplification.
View Article and Find Full Text PDFThis work describes the tailored design, green synthesis and characterization of noble metal (Pt, Ag and Au) nanoparticles (NPs) using Sapinduss Mukkorossi fruit extract (SMFE) and its signal NP collision signal response, based on the principle of the electrocatatlytic amplication (EA) method. Here, the SMFE can act as both the reducing and the capping agent for the fabrication of noble nanometals. The SMFE-capped NPs was available for the observation of a single NP collision signal.
View Article and Find Full Text PDFChitin and chitosan are biopolymers that have diverse applications in medicine, agriculture, food, cosmetics, pharmaceuticals, wastewater treatment and textiles. With bio-origins, they easily blend with biological systems and show exemplified compatibility which is mandatory when it comes to biomedical research. Chitin and chitosan are ecofriendly, however the processes that are used to recover them aren't ecofriendly.
View Article and Find Full Text PDFIn this work, a magneto-biosensor based on iron (II, III) oxide (magnetite, Fe₃O₄) nanoparticles for the detection of uric acid is developed and demonstrated. These Fe₃O₄ nanoparticles are successfully synthesized by a co-precipitation method comprising Fe and Fe with ammonium hydroxide, NH4OH, and using citric acid as a surfactant. Comparative studies of Fe₃O₄ nanoparticles with and without surfactant are also carried out to examine their characteristics.
View Article and Find Full Text PDFThe current generated by the collision of a single nanoparticle (NP) of palladium (Pd) on a gold (Au) ultramicroelectrode (UME) surface was observed using an electrocatalytic amplification method. The hydrogen peroxide reduction reaction was used for the electrocatalytic reaction because the hydrogen peroxide reduction reaction has no gas-phase product, which would induce rapid signal decay. The electrocatalytic current resulting from a single Pd nanoparticle on the Au UME shows a staircase response with accompanying slow current decay.
View Article and Find Full Text PDFA facile one-step, eco-friendly, and cost-effective approach for the formation of copper oxide (CuO) nanowires by a green method using saponin-rich fruit extract (SMFE). The physio-chemical characteristics of the synthesized CuO nanowires have been characterized by X-ray Diffractometry (XRD), X-ray Photoelectron Spectroscopy (XPS), FT-IR (Fourier Transform Infrared Spectroscopy, FE-SEM (Scanning Electron Microscopy), and High-Resolution Transmission Electron Microscopy (HR-TEM). Further, the electrocatalytic activity of the CuO nanowires synthesized with SMFE has been investigated, and they have been used as dopamine (DA) sensors.
View Article and Find Full Text PDFCollisions of silver nanoparticles (NPs) with a more electrocatalytic gold or platinum ultramicroelectrode (UME) surface have been observed by using an electrochemical method. Depending on the applied potential to the UME, the current response to the collision of Ag NPs on the UME resulted in various shape changes. A staircase decrease, a blip decrease, and a blip increase of the hydrazine oxidation current were obtained at an applied potential of 0.
View Article and Find Full Text PDFWe observed the collision of single Pt nanoparticles (NPs) onto an Au nanowire (NW) electrode by using electrocatalytic amplification. Previously, such observations had typically been performed by using a microscale disk-type ultramicroelectrode (UME). The use of a NW electrode decreased the background noise current and provided a shielding effect, owing to adsorption of the NPs onto the insulating sheath.
View Article and Find Full Text PDFSingle Pt nanoparticle (NP) collisions on an electrode surface were detected by using an electrocatalytic amplification method with a Pd ultramicroelectrode (UME). Pd is not a preferred material for UMEs for the detection of single Pt NP collisions, because Pd shows similar electrocatalytic activity compared with Pt for hydrazine oxidation, thus resulting in a high background current level. However, a Pt NP colliding on the Pd UME shows greatly enhanced activity compared with a Pt NP on an inert UME, such as a Au UME, which is usually used for the detection of single Pt NP collisions.
View Article and Find Full Text PDFThe current response of the collision of ascorbic acid-stabilized copper (Cu) single nanoparticles (NPs) on a gold (Au) ultramicroelectrode (UME) surface was observed by using an electrocatalytic amplification method. Here, the glucose oxidation electrocatalyzed by oxidized Cu NPs was used as the indicating reaction. In this system, the NP collision signals were obtained simultaneously by both direct particle electrolysis and electrocatalytic amplification.
View Article and Find Full Text PDFCatalytic properties of nanoparticles can be significantly enhanced by controlling nanoscale alloying and its structure. In this work, by using a facet-controlled Pt@Ni core-shell octahedron nanoparticle, we show that the nanoscale phase segregation can have directionality and be geometrically controlled to produce a Ni octahedron that is penetrated by Pt atoms along three orthogonal Cartesian axes and is coated by Pt atoms along its edges. This peculiar anisotropic diffusion of Pt core atoms along the ⟨100⟩ vertex, and then toward the ⟨110⟩ edges, is explained via the minimum strain energy for Ni-Ni pair interactions.
View Article and Find Full Text PDFCollisions of electrocatalytic platinum (Pt) single nanoparticles (NPs) with a less electrocatalytic nickel (Ni) ultramicroelectrode (UME) surface were detected by amplification of the current by electrocatalysis of NPs. Two typical types of current responses, a current staircase or blip (or spike), in single NP collision experiments were observed at a time with a new system consisting of Pt NP/Ni UME/hydrazine oxidation. The staircase current response was obtained when the collided NPs were attached to the electrode and continued to produce electrocatalytic current.
View Article and Find Full Text PDFPt-doping of an ultrathin Pd nanosheet results in the unprecedented structural rearrangement of a Pd nanosheet into a PdPt nanotent structure, in which a tripod stands on a triangular nanosheet. Further growth of Pt phase on this nanotent structure is dependent on the presence of surface-stabilizing CO molecules, leading to the formation of two distinct nanoscale phase segregated structures with respective structural features of a popped out Pt facet and an overgrown Pt layer.
View Article and Find Full Text PDFUltralong coaxial Au@Pt nanocables prepared by one-pot synthesis exhibit excellent electrocatalytic activity due to structural features of (1) numerous twinning boundaries and (2) lattice mismatch between the core and the shell.
View Article and Find Full Text PDFA fail-proof synthetic strategy has been developed for a multiply twinned dumbbell-shaped Rh@Pt nanostructure, which exhibits a superior electrocatalytic activity for methanol oxidation reaction. The unusually high electrocatalytic activity has been attributed to the synergistic effects of crystal twinning and core-shell structure.
View Article and Find Full Text PDFThe CO-assisted thermal decomposition of a new, surfactant-ligated Pt precursor, [Pt(acac)(NHR)](n) (n = 2, 3; R = C(18)H(37)), gives structurally uniform five-fold twinned Pt nanorods. The Pt nanorods, mostly covered by {100} facets, exhibit much enhanced electrocatalytic activity over {100} faceted Pt nanocubes, indicating the superior catalytic performance due to the presence of the reactive twinning interface.
View Article and Find Full Text PDFThis study demonstrates a highly sensitive sensing scheme for the detection of low concentrations of DNA, in principle down to the single biomolecule level. The previously developed technique of electrochemical current amplification for detection of single nanoparticle (NP) collisions at an ultramicroelectrode (UME) has been employed to determine DNA. The Pt NP/Au UME/hydrazine oxidation reaction was employed, and individual NP collision events were monitored.
View Article and Find Full Text PDFWe investigated the electrochemical detection of single iridium oxide nanoparticle (IrO(x) NP) collisions at the NaBH(4)-treated Pt ultramicroelectrode (UME) in a scanning electrochemical microscope (SECM) over an insulating surface. The NP collision events were monitored by observing the electrocatalytic water oxidation reaction at potentials where it does not take place on the Pt UME. These collisions occurred stochastically, resulting in a transient response ("blip") for each collision.
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