Advanced oxidation processes (AOPs) are the most efficient water cleaning technologies, but their applications face critical challenges in terms of mass/electron transfer limitations and catalyst loss/deactivation. Bipolar electrochemistry (BPE) is a wireless technique that is promising for energy and environmental applications. However, the synergy between AOPs and BPE has not been explored.
View Article and Find Full Text PDFImpact electrochemistry allows for the investigation of the properties of single entities, ranging from nanoparticles (NPs) to soft bio-particles. It has introduced a novel dimension in the field of biological analysis, enhancing researchers' ability to comprehend biological heterogeneity and offering a new avenue for developing novel diagnostic devices for quantifying biological analytes. This review aims to summarize the recent advancements in impact electrochemistry-based biosensing over the past two to three years and provide insights into the future directions of this field.
View Article and Find Full Text PDFAdvanced techniques for both environmental and biological prescription drug monitoring are of ongoing interest. In this work, a fluorescent sensor based on an Eu-doped anionic zinc-based metal-organic framework (Eu@Zn-MOF) was constructed for rapid visual analysis of the prescription drug molecule demecycline (DEM), achieving both high sensitivity and selectivity. The ligand 2-amino-[1,1'-biphenyl]-4,4'-dicarboxylic acid (bpdc-NH) not only provides stable cyan fluorescence (467 nm) for the framework through intramolecular charge transfer of bpdc-NH infinitesimal disturbanced by Zn but also chelates Eu, resulting in red (617 nm) fluorescence.
View Article and Find Full Text PDFNanomedicine is promising for disease prevention and treatment, but there are still many challenges that hinder its rapid development. A major challenge is to efficiently seek candidates with the desired therapeutic functions from tremendously available materials. Here, we report an integrated computational and experimental framework to seek alloy nanoparticles from the Materials Project library for antibacterial applications, aiming to learn the inverse screening concept from traditional medicine for nanomedicine.
View Article and Find Full Text PDFProtein kinase activity correlates closely with that of many human diseases. However, the existing methods for quantifying protein kinase activity often suffer from limitations such as low sensitivity, harmful radioactive labels, high cost, and sophisticated detection procedures, underscoring the urgent need for sensitive and rapid detection methods. Herein, we present a simple and sensitive approach for the homogeneous detection of protein kinase activity based on nanoimpact electrochemistry to probe the degree of aggregation of silver nanoparticles (AgNPs) before and after phosphorylation.
View Article and Find Full Text PDFPlasmon-enhanced electrochemistry (PEEC) has been observed to facilitate energy conversion systems by converting light energy to chemical energy. However, comprehensively understanding the PEEC mechanism remains challenging due to the predominant use of ensemble-based methodologies on macroscopic electrodes, which fails to measure electron-transfer kinetics due to constraints from mass transport and the averaging effect. In this study, we have employed nanoparticle impact electrochemistry (NIE), a newly developed electroanalytical technique capable of measuring electrochemical dynamics at a single-nanoparticle level under optimal mass transport conditions, along with microscopic electron-transfer theory for data interpretation.
View Article and Find Full Text PDFPrussian blue (PB) has emerged as a promising cathode material in aqueous batteries. It possesses two distinct redox centers, and the potassium ions (K ) are unevenly distributed throughout the compound, adding complexity to the interpretation of the K insertion/de-insertion kinetic mechanism. Traditional ensemble-averaged measurements are limited in uncovering the precise kinetic information of the PB particles, as the results are influenced by the construction of the porous composite electrode and the redox behavior from different particles.
View Article and Find Full Text PDFIn this work, we report a versatile and tunable platform for the construction of various cell array biochips using a simple soft lithographic approach to pattern polydopamine (PDA) arrays via microcontact printing (μCP). Instead of direct polymerization of PDA on the polydimethylsiloxane (PDMS) tips, dopamine monomers were first printed on the substrate followed by a self-oxidative polymerization step facilitated by ammonia vapor to grow PDA in situ, which greatly reduced the reaction time and prevented the PDMS tips from damaging. The improved robustness and utility of the PDMS tips allows the formation of tunable PDA array chips with controllable PDA feature size and shape.
View Article and Find Full Text PDFHomogeneous immunoassays represent an attractive alternative to traditional heterogeneous assays due to their simplicity and high efficiency. Homogeneous electrochemical assays, however, are not commonly accessed due to the requirement of electrode immobilization of the recognition elements. Herein, we demonstrate a new homogeneous electrochemical immunoassay based on the aggregation-collision strategy for the quantification of tumor protein biomarker alpha-fetoprotein (AFP).
View Article and Find Full Text PDFTumor protein quantification with high specificity, sensitivity, and efficiency is of great significance to enable early diagnosis and effective treatment. The existing methods for protein analysis usually suffer from high cost, time-consuming operation, and insufficient sensitivity, making them not clinically friendly. In this work, a label-free homogeneous sensor based on the nano-impact electroanalytic (NIE) technique was proposed for the detection of tumor protein marker alpha-fetoprotein (AFP).
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2022
Selective electrochemical production of valued chemicals is of significant importance but remains a great challenge in chemistry. Conventional approaches for enhancing reaction selectivity focus on the improvement of the catalysts themselves. In this work, we systematically studied the reaction kinetics and mass transport behavior of LaNiO nanocubes (LaNiO NCs) catalyzed hydrogen peroxide reduction reaction (HPRR) at ensemble and single nanoparticle levels using nano-impact electrochemistry (NIE).
View Article and Find Full Text PDFPlasmon enhanced electrochemistry (PEEC), where specific electrochemical reactions are promoted due to the reduced energy barrier of the reaction processes by the light excited "hot carriers" of the plasmonic nanoparticles, has aroused tremendous interest in recent years. A deep understanding of the PEEC process becomes a key issue for facilitating PEEC catalyst design and improving PEEC performance. This concept article begins with a brief discussion of the macroscopic electrochemical method of PEEC study of the plasmonic nanoparticle ensembles.
View Article and Find Full Text PDFThe structure-function relationship of plasmon-enhanced electrochemistry (PEEC) is of great importance for the design of efficient PEEC catalysts, but is rarely investigated at single nanoparticle level for the lack of an efficient nanoscale methodology. Herein, we report the utilization of nanoparticle impact electrochemistry to allow single nanoparticle PEEC, where the effect of incident light on the plasmonic Ag/Au nanoparticles for accelerating cobalt metal-organic framework nanosheets (Co-MOFNs) catalyzed hydrogen evolution reaction (HER) is systematically explored. It is found that the plasmon-excited hot carrier injection can lower the reaction activation energy, resulting in a much promoted reaction probability and the integral charge generated from individual collisions.
View Article and Find Full Text PDFThe classical size effect of Pt particles on oxygen reduction reaction (ORR) suggests that the activity and durability would decrease with reducing the particle size, self-limiting the effectiveness in maximizing the Pt utilization efficiency with the particle-size-reduction strategy. Herein, we discover an anomalous size effect based on Pt nanowires (NWs) with tunable diameters, where the monotonically increasing activity and durability for ORR were observed with decreasing the diameter from 2.4 to 1.
View Article and Find Full Text PDFIn recent years, nano-impact electrochemistry (NIE) has attracted widespread attention as a new electroanalytical approach for the analysis and characterization of single nanoparticles in solution. The accurate analysis of the large volume of the experimental data is of great significance in improving the reliability of this method. Unfortunately, the commonly used data analysis approaches, mainly based on manual processing, are often time-consuming and subjective.
View Article and Find Full Text PDFProtein quantification with high throughput and high sensitivity is essential in the early diagnosis and elucidation of molecular mechanisms for many diseases. Conventional approaches for protein assay often suffer from high costs, long analysis time, and insufficient sensitivity. The recently emerged nanoimpact electrochemistry (NIE), as a contrast, allows detection of analytes one at a time with simplicity, fast response, high throughput, and the potential of reducing the detection limits down to the single entity level.
View Article and Find Full Text PDFElectrocatalytic water splitting holds great promise for renewable energy conversion and storage systems. However, it usually suffers from sluggish kinetics, which greatly hinders its real application. Here, we demonstrate the utilization of the localized surface plasmon resonance (LSPR) of Au nanorods (AuNRs) to significantly improve the electroactivity of both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) at Co-MOF nanosheets (Co-MOFNs) under different polarizations.
View Article and Find Full Text PDFWe for the first time propose a new concept where a greater enhancement in dual potential electrochemiluminescence (ECL) of a single graphene quantum dot (GQD) emitter can be achieved through the coupling between chemical and electrochemical reactions of two different coreactants of KSO and NaSO.
View Article and Find Full Text PDFA chip-based approach for electrochemical characterization and detection of microsomes and exosomes based on direct electro-oxidation of metal nanoparticles (MNPs) that specifically recognize surface markers of these vesicles is reported. It is found that exosomes and microsomes derived from prostate cancer cells can be identified by their surface proteins EpCAM and PSMA, suggesting the potential of exosomes and microsomes for use as diagnostic biomarkers.
View Article and Find Full Text PDFThe electrochemical detection of nucleic acids using an electrocatalytic reporter system and nanostructured microelectrodes is a powerful approach to ultrasensitive biosensing. In this report we systematically study for the first time the behavior of an electrocatalytic reporter system at nucleic acid-modified electrodes with varying structures and sizes. [Ru(NH3)6](3+) is used as a primary electron acceptor that is electrostatically attracted to nucleic acid-modified electrodes, and [Fe(CN)6](3-) is introduced into the redox system as a secondary electron acceptor to regenerate Ru(3+) after electrochemical reduction.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
November 2014
Circulating tumor cells (CTCs) can be collected noninvasively and provide a wealth of information about tumor phenotype. For this reason, their specific and sensitive detection is of intense interest. Herein, we report a new, chip-based strategy for the automated analysis of cancer cells.
View Article and Find Full Text PDFPhys Chem Chem Phys
January 2013
The kinetics of proton reduction are reported for Ni and NiO surfaces and compared to that measured at Ni@NiO nanoparticles. Kinetic acceleration is found to occur by virtue of oxide overlayers and not due to size effects on the nanoscale.
View Article and Find Full Text PDFThe electro-oxidation of silver and nickel nanoparticles in aqueous solution was studied via their collisions with a carbon electrode. The average charge passed per impact varies with electrode potential and was analysed to determine that AgNPs display an electrochemically fast ("reversible") one-electron oxidation, whilst the NiNPs exhibit slow ("irreversible") 2-electron kinetics. Kinetic parameters are reported.
View Article and Find Full Text PDFThe use of particle-impact coulometry in identifying and quantifying nanoparticles tagged (or labelled) with electroactive molecules is demonstrated via the detection of 1,4-nitrothiophenol-tagged silver nanoparticles in aqueous dispersion at potentials more negative than -0.17 V (vs. Ag/AgCl, the reduction potential of nitrothiophenol) via monitoring of particle-electrode collisions.
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