Electrochemiluminescence (ECL) is a widely used analytical technique with the advantages of high sensitivity and low background signal. The recent and rapid development of electrochemical materials, luminophores, and optical elements significantly increases the ECL signals and, thus, ECL imaging with enhanced spatial and temporal resolutions is realized. Currently, ECL imaging is successfully applied to high-throughput bioanalysis and to visualize the distribution of molecules at single cells. Compared with other optical bioassays, no optical excitation is involved in imaging, so the approach avoids a background signal from illumination and increases the detection sensitivity. This review highlights some of the most exciting developments in this field, including the mechanisms, electrode designs, and the applications of ECL imaging in bioanalysis and at single cells and particles.

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.

Herein, a single biomolecule is imaged by electrochemiluminescence (ECL) using Ru­(bpy)3 2+-doped silica/Au nanoparticles (RuDSNs/AuNPs) as the ECL nanoemitters. The ECL emission is confined to the local surface of RuDSNs leading to a significant enhancement in the intensity. To prove the concept, a single protein molecule at the electrode is initially visualized using the as-prepared RuDSN/AuNPs nanoemitters. Furthermore, the nanoemitter-labeled antibody is linked at the cellular membrane to image a single membrane protein at one cell, without the interference of current and optical background. The success in single-biomolecule ECL imaging solves the long-lasting task in the ultrasensitive ECL analysis, which should be able to provide more elegant information about the protein in cellular biology.

White NM, Jiang D, Burgess JD, Bederman IR, Previs SF, Kelley TJ. Altered cholesterol homeostasis in cultured and in vivo models of cystic fibrosis.