The testing and evaluation of catalysts in CO electroreduction is a very tedious process. To study the catalytic system of CO reduction more quickly and efficiently, it is necessary to establish a method that can detect multiple catalysts at the same time. Herein, a series of CuBi bimetallic catalysts have been successfully prepared on a single glass carbon electrode by a scanning micropieptte contact method.
View Article and Find Full Text PDFElectrochemical CO reduction has garnered significant interest in the conversion of sustainable energy to valuable fuels and chemicals. Cu-based bimetallic catalysts play a crucial role in enhancing CO concentration on Cu sites for efficient C─C coupling reactions, particularly for C product generation. To enhance Cu's electronic structure and direct its selectivity toward C products, a novel strategy is proposed involving the in situ electropolymerization of a nano-thickness cobalt porphyrin polymeric network (EP-CoP) onto a copper electrode, resulting in the creation of a highly effective EP-CoP/Cu tandem catalyst.
View Article and Find Full Text PDFTwo challenges should be overcome for the ultra-precision machining of micro-optical element with freeform curved surface: one is the intricate geometry, the other is the hard-to-machining optical materials due to their hardness, brittleness or flexibility. Here scanning electrochemical probe lithography (SECPL) is developed, not only to meet the machining need of intricate geometry by 3D direct writing, but also to overcome the above mentioned mechanical properties by an electrochemical material removal mode. Through the electrochemical probe a localized anodic voltage is applied to drive the localized corrosion of GaAs.
View Article and Find Full Text PDFEnhancing the electrochemical activity of graphene holds great significance for expanding its applications in various electrochemistry fields. In this study, we have demonstrated a facile and quantitative approach for modulating the defect density of single-layer graphene (SLG) an electrochemically induced bromination process facilitated by cyclic voltammetry. This controlled defect engineering directly impacts the heterogeneous electron transfer (HET) rate of SLG.
View Article and Find Full Text PDFIn nature and technologies, many chemical reactions occur at interfaces with dimensions approaching that of a single reacting species in nano- and angstrom-scale. Mechanisms governing reactions at this ultimately small spatial regime remain poorly explored because of challenges to controllably fabricate required devices and assess their performance in experiment. Here we report how efficiency of electrochemical reactions evolves for electrodes that range from just one atom in thickness to sizes comparable with and exceeding hydration diameters of reactant species.
View Article and Find Full Text PDFElectrochemical nanoimprint lithography (ECNL) has emerged as a promising technique for fabricating three-dimensional micro/nano-structures (3D-MNSs) directly on semiconductor wafers. This technique is based on a localized corrosion reaction induced by the contact potential across the metal/semiconductor boundaries. The anodic etching of semiconductor and the cathodic reduction of electron acceptors occur at the metal/semiconductor/electrolyte interface and the Pt mold surface, respectively.
View Article and Find Full Text PDFElectrocatalytic CO reduction reaction (CO RR) based on molecular catalysts, for example, cobalt porphyrin, is promising to enhance the carbon cycle and mitigate current climate crisis. However, the electrocatalytic performance and accurate evaluations remain problems because of either the low loading amount or the low utilization rate of the electroactive CoN sites. Herein a monomer is synthesized, cobalt(II)-5,10,15,20-tetrakis(3,5-di(thiophen-2-yl)phenyl)porphyrin (CoP), electropolymerized onto carbon nanotubes (CNTs) networks, affording a molecular electrocatalyst of 3D microporous nanofilm (EP-CoP, 2-3 nm thickness) with highly dispersed CoN sites.
View Article and Find Full Text PDFAdvanced Ag nanoparticles (Ag NPs) were prepared by wet chemical oxidation-reduction method, using mainly the tannic acid as reducing agent and carboxymethylcellulose sodium as stabilizer. The prepared Ag NPs uniformly disperse and are stable for more than one month without agglomeration. The studies of transmission electron microscopy (TEM) and ultraviolet-visible (UV-vis) absorption spectroscopy indicate that the Ag NPs are in homogeneous sphere with only 4.
View Article and Find Full Text PDFAs a semimetal with a zero band gap and single-atom-scale thickness, single layer graphene (SLG) has excellent electron conductivity on its basal plane. If the band gap could be opened and regulated controllably, SLG would behave as a semiconductor. That means electronic elements or even electronic circuits with single-atom thickness could be expected to be printed on a wafer-scale SLG substrate, which would bring about a revolution in Moore's law of integrated circuits, not by decreasing the feature size of line width, but by piling up the atomic-scale-thickness of an SLG circuit board layer by layer.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
March 2023
Proton transfer is crucial for electrocatalysis. Accumulating cations at electrochemical interfaces can alter the proton transfer rate and then tune electrocatalytic performance. However, the mechanism for regulating proton transfer remains ambiguous.
View Article and Find Full Text PDFAqueous zinc-metal batteries have attracted extensive attention due to their outstanding merits of high safety and low cost. However, the intrinsic thermodynamic instability of zinc in aqueous electrolyte inevitably results in hydrogen evolution, and the consequent generation of OH at the interface will dramatically exacerbate the formation of dead zinc and dendrites. Herein, a dynamically interfacial pH-buffering strategy implemented by N-methylimidazole (NMI) additive is proposed to remove the detrimental OH at zinc/electrolyte interface in real-time, thus eliminating the accumulation of by-products fundamentally.
View Article and Find Full Text PDFMetal-organic frames (MOFs) have recently been used to support redox enzymes for highly sensitive and selective chemical sensors for small biomolecules such as oxygen (O), hydrogen peroxide (HO), etc. However, most MOFs are insulative and their three-dimensional (3D) porous structures hinder the electron transfer pathway between the current collector and the redox enzyme molecules. In order to facilitate electron transfer, here we adopt two-dimensional (2D) metal-organic layers (MOLs) to support the HRP molecules in the detection of HO.
View Article and Find Full Text PDFIf hydrogen can be stored and carried safely at a high density, hydrogen-fuel cells offer effective solutions for vehicles. The stable chemisorption of atomic hydrogen on single layer graphene (SLG) seems a perfect solution in this regard, with a theoretical maximum storage capacity of 7.7 wt %.
View Article and Find Full Text PDFSolid/liquid interfacial structure occupies great importance in chemistry, biology, and materials. In this paper, by combining EC-SERS study and DFT calculation, we reveal the adsorption and dimerization of sulfite (SO) at a gold electrode/water solution interface, and establish an adsorption displacement strategy to suppress the dimerization of sulfite. At the gold electrode/sodium sulfite solution interface, at least two layers of SO anions are adsorbed on the electrode surface.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
November 2020
Scanning electrochemical microscopy (SECM) is one of the most important instrumental methods of modern electrochemistry due to its high spatial and temporal resolution. We introduced SECM into nanomachining by feeding the electrochemical modulations of the tip electrode back to the positioning system, and we demonstrated that SECM is a versatile nanomachining technique on semiconductor wafers using electrochemically induced chemical etching. The removal profile was correlated to the applied tip current when the tip was held stationary and when it was moving slowly (<20 μm s ), and it followed Faraday's law.
View Article and Find Full Text PDFThe rational design and applications of plasmon-mediated chemical reactions (PMCRs) are fundamentally determined by an understanding of photon-electron-molecule interactions. However, the current understanding of the PMCR of plasmon-decayed hot electron-mediated reactions remains implicit, since there has not been a single measurement of both hot-electron transfer and molecular transformation following photon excitation. Therefore, we invented a method called microphotoelectrochemical surface-enhanced Raman spectroscopy (μPEC-SERS) that uses an ultramicroelectrode (UME) whose dimensions match those of the focused laser spot.
View Article and Find Full Text PDFHere we propose a strategy of radical oxidation reaction for the high-efficiency production of graphene oxide (GO). GO plays important roles in the sustainable development of energy and the environment, taking advantages of oxygen-containing functional groups for good dispersibility and assembly. Compared with Hummers' method, electrochemical exfoliation of graphite is considered facile and green, although the oxidation is fairly low.
View Article and Find Full Text PDFThe interfacial electron transfer capability of Si/SiO2 wafer supported single layer graphene is optimized by thermal annealing in an inert gas environment, which facilitates its applications in both electrochemical and electronic devices.
View Article and Find Full Text PDFHere we report photoelectric-effect-enhanced interfacial charge transfer reactions. The electrochemical corrosion rate of n-type gallium arsenide (n-GaAs) induced by the contact potential at platinum (Pt) and GaAs boundaries can be accelerated by the photoelectric effect of n-GaAs. When a GaAs wafer is illuminated with a xenon light source, the electrons in the valence band of GaAs will be excited to the conduction band and then move to the Pt boundaries due to the different work functions of the two materials.
View Article and Find Full Text PDFWe propose programed potential modulation strategies to balance the ion intercalation/deintercalation, surface tailoring and bubbling dispersion processes in the electrochemical exfoliation of graphite, resulting in high-quality graphene with high crystallinity, low oxidation degree, uniform size distribution and few layers.
View Article and Find Full Text PDFRecently, the photoelectric effect in metals in electrolyte environments has aroused the interest of researchers. However, direct evidence for surface plasmons-enhanced electrochemical reactions involving classic outer-sphere reactions of reversible redox couples is seldom reported. We used a surface plasmons-active gold-mushroom-array as a working electrode and observed enhanced faradaic current from ferrocenemethanol following illumination with a xenon lamp.
View Article and Find Full Text PDFThe functional three dimensional micro-nanostructures (3D-MNS) play crucial roles in integrated and miniaturized systems because of the excellent physical, mechanical, electric and optical properties. Nanoimprint lithography (NIL) has been versatile in the fabrication of 3D-MNS by pressing thermoplastic and photocuring resists into the imprint mold. However, direct nanoimprint on the semiconductor wafer still remains a great challenge.
View Article and Find Full Text PDFNanoelectrodes, with dimensions below 100 nm, have the advantages of high sensitivity and high spatial resolution. These electrodes have attracted increasing attention in various fields such as single cell analysis, single-molecule detection, single particle characterization and high-resolution imaging. The rapid growth of novel nanoelectrodes and nanoelectrochemical methods brings enormous new opportunities in the field.
View Article and Find Full Text PDFAlthough metal assisted chemical etching (MacEtch) has emerged as a versatile micro-nanofabrication method for semiconductors, the chemical mechanism remains ambiguous in terms of both thermodynamics and kinetics. Here we demonstrate an innovative phenomenon, , the contact electrification between platinum (Pt) and an n-type gallium arsenide (100) wafer (n-GaAs) can induce interfacial redox reactions. Because of their different work functions, when the Pt electrode comes into contact with n-GaAs, electrons will move from n-GaAs to Pt and form a contact electric field at the Pt/n-GaAs junction until their electron Fermi levels () become equal.
View Article and Find Full Text PDF