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  Angstrom-resolved real-time dissection of electrochemically active noble metal interfaces

Shrestha, B. R., Baimpos, T., Raman, S., & Valtiner, M. (2014). Angstrom-resolved real-time dissection of electrochemically active noble metal interfaces. ACS Nano, 8(6), 5979-5987. doi:10.1021/nn501127n.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-0026-B45F-8 Version Permalink: http://hdl.handle.net/11858/00-001M-0000-0026-B460-2
Genre: Journal Article

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 Creators:
Shrestha, Buddha R.1, Author              
Baimpos, Theodoros1, Author              
Raman, Sangeetha1, Author              
Valtiner, Markus1, Author              
Affiliations:
1Interaction Forces and Functional Materials, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society, ou_1863357              

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Free keywords: Catalysis; Corrosion; Liquids; Metallic compounds; Metals; Optical properties; Precious metals; Bioelectrochemical process; Electrochemical reactions; Electrochemical surfaces; electrochemisty; Oxide growth; Technological applications; Visualization of dynamic process; White-light interferometry
 Abstract: Electrochemical solid/liquid interfaces are critically important for technological applications and materials for energy storage, harvesting, and conversion. Yet, a real-time Angstrom-resolved visualization of dynamic processes at electrified solid liquid interfaces has not been feasible. Here we report a unique real-time atomistic view into dynamic processes at electrochemically active metal interfaces using white light interferometry in an electrochemical surface forces apparatus. This method allows simultaneous deciphering of both sides of an electrochemical interface-the solution and the metal side-with microsecond resolution under dynamically evolving reactive conditions that are inherent to technological systems in operando. Quantitative in situ analysis of the potentiodynamic electrochemical oxidation/reduction of noble metal surfaces shows that Angstrom thick oxides formed on Au and Pt are high-ik materials; that is, they are metallic or highly defect-rich semiconductors, while Pd forms a low-ik oxide. In contrast, under potentiostatic growth conditions, all noble metal oxides exhibit a low-ik behavior. On the solution side, we reveal hitherto unknown strong electrochemical reaction forces, which are due to temporary charge imbalance in the electric double layer caused by depletion/generation of charged species. The real-time capability of our approach reveals significant time lags between electron transfer, oxide reduction/oxidation, and solution side reaction during a progressing electrode process. Comparing the kinetics of solution and metal side responses provides evidence that noble metal oxide reduction proceeds via a hydrogen adsorption and subsequent dissolution/redeposition mechanism. The presented approach may have important implications for designing emerging materials utilizing electrified interfaces and may apply to bioelectrochemical processes and signal transmission.

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Language(s): eng - English
 Dates: 2014-06-24
 Publication Status: Published in print
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Method: -
 Identifiers: ISI: 000338089200062
DOI: 10.1021/nn501127n
 Degree: -

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Title: ACS Nano
Source Genre: Journal
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Affiliations:
Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 8 (6) Sequence Number: - Start / End Page: 5979 - 5987 Identifier: Other: 1936-0851
CoNE: https://pure.mpg.de/cone/journals/resource/1936-0851