Chuhong Lin

New Insights into Fundamental Electron Transfer from Single Nanoparticle Voltammetry

The reductive redox behavior of oxygen in aqueous acid solution leading first to adsorbed superoxide species at single palladium coated multiwalled carbon nanotubes (of length ca. 5 μm and width 130 nm) is reported. The small dimensions of the electroactive surface create conditions of high mass-transport permitting the resolution of electrode kinetic effects. In combination with new theoretical models, it is shown that the physical location of the formed product within the double layer of the electrode profoundly influences the observed electron transfer kinetics. This generically important result gives new physical insights into the modeling of the many electrochemical processes involving adsorbed intermediates.

Coupled Optical and Electrochemical Probing of Silver Nanoparticle Destruction in a Reaction Layer

Abstract The oxidation of silver nanoparticles is induced to occur near to, but not at, an electrode surface. This reaction at a distance from the electrode is studied through the use of dark‐field microscopy, allowing individual nanoparticles and their reaction with the electrode product to be visualized. The oxidation product diffuses away from the electrode and oxidizes the nanoparticles in a reaction layer, resulting in their destruction. The kinetics of the silver nanoparticle solution‐phase reaction is shown to control the length scale over which the nanoparticles react. In general, the new methodology offers a route by which nanoparticle reactivity can be studied close to an electrode surface.

Electrochemistry of Single Enzymes: Fluctuations of Catalase Activities

Dynamic fluctuations of the catalytic ability of single catalase enzymes toward hydrogen peroxide decomposition are observed via the nanoimpact technique. The electrochemical signals of single enzymes show that the catalytic ability of single enzymes can temporarily be much higher than expected from the classical, time-averaged Michaelis-Menten description. By combination of experimental data with a new theoretical model, we interpret the unusual enhancement of the single catalase signal and find that single catalases show large fluctuations of the catalytic ability.