Electrochemiluminescence (ECL)-based
capacitance microscopy using
a square-wave voltage is established unprecedentedly to realize the
label-free visualization of species on electrode surfaces and cellular
plasma membranes. The drop in the local capacitance upon the binding
of species to the surface or to a cellular membrane is derived to
induce a relatively larger potential drop (V
dl) across the double layer on the local electrode surface,
which is utilized to prompt enhanced ECL at the binding position.
The square-wave voltage with a frequency of as high as 1.5 kHz is
proven to be favorable for the discrimination of the local ECL from
the surrounding signal. Using this new detection principle and resultant
capacitance microscopy, carcinoembryonic antigens (CEA) at amounts
of as low as 1 pg can be visualized. Further application of this approach
permits the direct imaging of CEA antigens on single MCF-7 cells through
the capacitance change after the formation of the antigen–antibody
complex. Successful visualization of the analyte without any ECL tag
will allow not only special capacitance microscopy for label-free
bioassays but also a novel ECL detection approach for the sensitive
detection of biomolecules.
Electrocatalysis is dominated by reaction at the solid–liquid–gas interface; surface properties of electrocatalysts determine the electrochemical behavior. The surface charge of active sites on catalysts modulate adsorption and desorption of intermediates. However, there is no direct evidence to bridge surface charge and catalytic activity of active sites. Defects (active sites) were created on a HOPG (highly oriented pyrolytic graphite) surface that broke the intrinsic sp2‐hybridization of graphite by plasma, inducing localization of surface charge onto defective active sites, as shown by scanning ion conductance microscopy (SICM) and Kelvin probe force microscopy (KPFM). An electrochemical test revealed enhanced intrinsic activity by the localized surface charge. DFT calculations confirmed the relationship between surface charge and catalytic activity. This work correlates surface charge and catalytic activity, providing insights into electrocatalytic behavior and guiding the design of advanced electrocatalysts.
This work reveals the mechanism of CO2 electrochemical reduction on ligand-protected Au nanoclusters and catalytic sites responsible for increased selectivity towards CO.
Anodic TiO2 nanotubes have been studied extensively for many years. However, the growth kinetics still remains unclear. The systematic study of the current transient under constant anodizing voltage has not been mentioned in the original literature. Here, a derivation and its corresponding theoretical formula are proposed to overcome this challenge. In this paper, the theoretical expressions for the time dependent ionic current and electronic current are derived to explore the anodizing process of Ti. The anodizing current-time curves under different anodizing voltages and different temperatures are experimentally investigated in the anodization of Ti. Furthermore, the quantitative relationship between the thickness of the barrier layer and anodizing time, and the relationships between the ionic/electronic current and temperatures are proposed in this paper. All of the current-transient plots can be fitted consistently by the proposed theoretical expressions. Additionally, it is the first time that the coefficient A of the exponential relationship (ionic current j(ion) = A exp(BE)) has been determined under various temperatures and voltages. And the results indicate that as temperature and voltage increase, ionic current and electronic current both increase. The temperature has a larger effect on electronic current than ionic current. These results can promote the research of kinetics from a qualitative to quantitative level.
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