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Stochastic Analysis of Electron Transfer and Mass Transport in Confined Solid/Liquid Interfaces

Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Institute for Solar Fuels, Hahn-Meitner-Platz 1, D-14109 Berlin, Germany
Surfaces 2020, 3(3), 392-407; https://doi.org/10.3390/surfaces3030029
Received: 6 July 2020 / Revised: 3 August 2020 / Accepted: 5 August 2020 / Published: 8 August 2020
Molecular-level understanding of electrified solid/liquid interfaces has recently been enabled thanks to the development of novel in situ/operando spectroscopic tools. Among those, ambient pressure photoelectron spectroscopy performed in the tender/hard X-ray region and coupled with the “dip and pull” method makes it possible to simultaneously interrogate the chemical composition of the interface and built-in electrical potentials. On the other hand, only thin liquid films (on the order of tens of nanometers at most) can be investigated, since the photo-emitted electrons must travel through the electrolyte layer to reach the photoelectron analyzer. Due to the challenging control and stability of nm-thick liquid films, a detailed experimental electrochemical investigation of such thin electrolyte layers is still lacking. This work therefore aims at characterizing the electrochemical behavior of solid/liquid interfaces when confined in nanometer-sized regions using a stochastic simulation approach. The investigation was performed by modeling (i) the electron transfer between a solid surface and a one-electron redox couple and (ii) its diffusion in solution. Our findings show that the well-known thin-layer voltammetry theory elaborated by Hubbard can be successfully applied to describe the voltammetric behavior of such nanometer-sized interfaces. We also provide an estimation of the current densities developed in these confined interfaces, resulting in values on the order of few hundreds of nA·cm−2. We believe that our results can contribute to the comprehension of the physical/chemical properties of nano-interfaces, thereby aiding to a better understanding of the capabilities and limitations of the “dip and pull” method. View Full-Text
Keywords: in situ ambient pressure XPS; dip and pull; confined solid/liquid interface; thin-film voltammetry; Hubbard’s model; nano-interfaces in situ ambient pressure XPS; dip and pull; confined solid/liquid interface; thin-film voltammetry; Hubbard’s model; nano-interfaces
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Favaro, M. Stochastic Analysis of Electron Transfer and Mass Transport in Confined Solid/Liquid Interfaces. Surfaces 2020, 3, 392-407.

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