Mass Transport and Electron Transfer at the Electrochemical-Confined Interface

Abstract

Single entity measurements based on the stochastic collision electrochemistry provide a promising and versatile means to study single molecules, single particles, single droplets, etc. Conceptually, mass transport and electron transfer are the two main processes at the electrochemically confined interface that underpin the most transient electrochemical responses resulting from the stochastic and discrete behaviors of single entities at the microscopic scale. This perspective demonstrates how to achieve controllable stochastic collision electrochemistry by effectively altering the two processes. Future challenges and opportunities for stochastic collision electrochemistry are also highlighted.

Formation of Molecular Junctions by Single-Entity Collision Electrochemistry

“…This methodology involves the deliberate manipulation of individual molecules or nanoparticles (NPs) through stochastic collisions, thereby facilitating meticulous fabrication and comprehensive characterization of nanostructures. 30 Within a typical NP collision experiment, with molecules modified on the surfaces of a tethered electrode (substrate) or the free moving NP or both, each collision event represents an opportunity to generate single or few molecules linked junctions. The formed NPs−molecules−substrate architectures can have immediate or enduring significance in the study of molecule dynamics at the nanoscale and, in a broader context, could be regarded as a novel molecular junction, colliding molecular junctions.…”

“…15,73 In a classic electrochemical reaction, mass/charge transport is a preliminary process that is followed by the electron transfer at the electrode/electrolyte interface. 30 SECE measurement has been successfully applied to identify and quantify the mass transport (particles, charged ions, etc.) and charge transfer through a molecule junction in real time.…”

“…Like the break junction method, SECE offers the ability to dynamically create transient or permanent molecular junctions. This methodology involves the deliberate manipulation of individual molecules or nanoparticles (NPs) through stochastic collisions, thereby facilitating meticulous fabrication and comprehensive characterization of nanostructures . Within a typical NP collision experiment, with molecules modified on the surfaces of a tethered electrode (substrate) or the free moving NP or both, each collision event represents an opportunity to generate single or few molecules linked junctions.…”

“…Mass/charge transport and charge transfer are at the center of control electrochemical properties in electrosynthesis, catalysis, and energy storage and transformation devices. , In a classic electrochemical reaction, mass/charge transport is a preliminary process that is followed by the electron transfer at the electrode/electrolyte interface . SECE measurement has been successfully applied to identify and quantify the mass transport (particles, charged ions, etc.)…”

Phase-Resolved Electrochemiluminescence with a Single Luminophore

“…Electrogenerated chemiluminescence (ECL) is a process by which a redox reaction gives rise to photon emission without the need for incident light . Both aqueous and organic luminophores are widely used in a range of applications in biology, sensing devices, and phase boundary determination. , Moreover, all radical intermediates are generated at the surface of the electrode; this process is confined within a couple of micrometers of the surface. − …”