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Title: Adsorption of Molecular Nitrogen in Electrical Double Layers near Planar and Atomically Sharp Electrodes

Abstract

Here, the adsorption of gas molecules at electrode–electrolyte interfaces is an important step in electrochemical reactions. Using molecular dynamics simulations, we investigate the adsorption of dissolved N 2 in the electrical double layers (EDLs) of an aqueous electrolyte near planar and 1 nm radius spherical carbon electrodes. The adsorption of N 2 is found to be overall enriched near neutral electrodes regardless of their surface curvature, although it can be locally enriched or depleted depending on the distance from the electrode surface. In comparison, the adsorption of N 2 in the EDL near negatively charged electrodes is found to increase under a moderate surface charge density, but decrease under a high surface charge density, especially near a planar electrode. By analyzing the potential of mean force for dissolved N 2, the solvent-induced effects are found to play important roles in influencing the adsorption of N 2 in the EDLs. The adsorption behavior of N 2 molecules, especially their dependence on the surface charge and curvature of electrodes, is further rationalized by examining the structure of interfacial water molecules, their interference with the hydration shell of N 2, and their modification by the electrification of electrodes.

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1484108
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Langmuir
Additional Journal Information:
Journal Name: Langmuir; Journal ID: ISSN 0743-7463
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING

Citation Formats

Zhang, Fei, Yu, Zhou, Rondinone, Adam J., Huang, Jingsong, Sumpter, Bobby G., and Qiao, Rui. Adsorption of Molecular Nitrogen in Electrical Double Layers near Planar and Atomically Sharp Electrodes. United States: N. p., 2018. Web. doi:10.1021/acs.langmuir.8b03161.
Zhang, Fei, Yu, Zhou, Rondinone, Adam J., Huang, Jingsong, Sumpter, Bobby G., & Qiao, Rui. Adsorption of Molecular Nitrogen in Electrical Double Layers near Planar and Atomically Sharp Electrodes. United States. doi:10.1021/acs.langmuir.8b03161.
Zhang, Fei, Yu, Zhou, Rondinone, Adam J., Huang, Jingsong, Sumpter, Bobby G., and Qiao, Rui. Fri . "Adsorption of Molecular Nitrogen in Electrical Double Layers near Planar and Atomically Sharp Electrodes". United States. doi:10.1021/acs.langmuir.8b03161.
@article{osti_1484108,
title = {Adsorption of Molecular Nitrogen in Electrical Double Layers near Planar and Atomically Sharp Electrodes},
author = {Zhang, Fei and Yu, Zhou and Rondinone, Adam J. and Huang, Jingsong and Sumpter, Bobby G. and Qiao, Rui},
abstractNote = {Here, the adsorption of gas molecules at electrode–electrolyte interfaces is an important step in electrochemical reactions. Using molecular dynamics simulations, we investigate the adsorption of dissolved N2 in the electrical double layers (EDLs) of an aqueous electrolyte near planar and 1 nm radius spherical carbon electrodes. The adsorption of N2 is found to be overall enriched near neutral electrodes regardless of their surface curvature, although it can be locally enriched or depleted depending on the distance from the electrode surface. In comparison, the adsorption of N2 in the EDL near negatively charged electrodes is found to increase under a moderate surface charge density, but decrease under a high surface charge density, especially near a planar electrode. By analyzing the potential of mean force for dissolved N2, the solvent-induced effects are found to play important roles in influencing the adsorption of N2 in the EDLs. The adsorption behavior of N2 molecules, especially their dependence on the surface charge and curvature of electrodes, is further rationalized by examining the structure of interfacial water molecules, their interference with the hydration shell of N2, and their modification by the electrification of electrodes.},
doi = {10.1021/acs.langmuir.8b03161},
journal = {Langmuir},
number = ,
volume = ,
place = {United States},
year = {Fri Nov 09 00:00:00 EST 2018},
month = {Fri Nov 09 00:00:00 EST 2018}
}

Journal Article:
Free Publicly Available Full Text
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