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Title: Unravelling the electrochemical double layer by direct probing of the solid/liquid interface

Abstract

The electrochemical double layer plays a critical role in electrochemical processes. Whilst there have been many theoretical models predicting structural and electrical organization of the electrochemical double layer, the experimental verification of these models has been challenging due to the limitations of available experimental techniques. The induced potential drop in the electrolyte has never been directly observed and verified experimentally, to the best of our knowledge. In this study, we report the direct probing of the potential drop as well as the potential of zero charge by means of ambient pressure X-ray photoelectron spectroscopy performed under polarization conditions. By analyzing the spectra of the solvent (water) and a spectator neutral molecule with numerical simulations of the electric field, we discern the shape of the electrochemical double layer profile. In addition, we determine how the electrochemical double layer changes as a function of both the electrolyte concentration and applied potential.

Authors:
 [1];  [1];  [2];  [3];  [1];  [1];  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis (JCAP)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1377433
Grant/Contract Number:  
AC02-05CH11231; SC0004993
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; electrochemistry; surface spectroscopy; surfaces, interfaces and thin films

Citation Formats

Favaro, Marco, Jeong, Beomgyun, Ross, Philip N., Yano, Junko, Hussain, Zahid, Liu, Zhi, and Crumlin, Ethan J. Unravelling the electrochemical double layer by direct probing of the solid/liquid interface. United States: N. p., 2016. Web. doi:10.1038/ncomms12695.
Favaro, Marco, Jeong, Beomgyun, Ross, Philip N., Yano, Junko, Hussain, Zahid, Liu, Zhi, & Crumlin, Ethan J. Unravelling the electrochemical double layer by direct probing of the solid/liquid interface. United States. https://doi.org/10.1038/ncomms12695
Favaro, Marco, Jeong, Beomgyun, Ross, Philip N., Yano, Junko, Hussain, Zahid, Liu, Zhi, and Crumlin, Ethan J. Wed . "Unravelling the electrochemical double layer by direct probing of the solid/liquid interface". United States. https://doi.org/10.1038/ncomms12695. https://www.osti.gov/servlets/purl/1377433.
@article{osti_1377433,
title = {Unravelling the electrochemical double layer by direct probing of the solid/liquid interface},
author = {Favaro, Marco and Jeong, Beomgyun and Ross, Philip N. and Yano, Junko and Hussain, Zahid and Liu, Zhi and Crumlin, Ethan J.},
abstractNote = {The electrochemical double layer plays a critical role in electrochemical processes. Whilst there have been many theoretical models predicting structural and electrical organization of the electrochemical double layer, the experimental verification of these models has been challenging due to the limitations of available experimental techniques. The induced potential drop in the electrolyte has never been directly observed and verified experimentally, to the best of our knowledge. In this study, we report the direct probing of the potential drop as well as the potential of zero charge by means of ambient pressure X-ray photoelectron spectroscopy performed under polarization conditions. By analyzing the spectra of the solvent (water) and a spectator neutral molecule with numerical simulations of the electric field, we discern the shape of the electrochemical double layer profile. In addition, we determine how the electrochemical double layer changes as a function of both the electrolyte concentration and applied potential.},
doi = {10.1038/ncomms12695},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {Wed Aug 31 00:00:00 EDT 2016},
month = {Wed Aug 31 00:00:00 EDT 2016}
}

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