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Title: Insight into hydrogen production through molecular simulation of an electrode-ionomer electrolyte system

Abstract

In this work, we examine metal electrode-ionomer electrolyte systems at high voltage (negative surface charge) and at high pH to assess factors that influence hydrogen production efficiency. We simulate the hydrogen evolution electrode interface investigated experimentally in the work of Bates et al. [J. Phys. Chem. C 119, 5467 (2015)] using a combination of first principles calculations and classical molecular dynamics. With this detailed molecular information, we explore the hypotheses posed in the work of Bates et al. In particular, we examine the response of the system to increased bias voltage and oxide coverage in terms of the potential profile, changes in solvation and species concentrations away from the electrode, surface concentrations, and orientation of water at reactive surface sites. Finally, we discuss this response in the context of hydrogen production.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]
  1. Sandia National Lab. (SNL-CA), Livermore, CA (United States)
  2. Northeastern Univ., Boston, MA (United States)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-CA), Livermore, CA (United States); Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office
OSTI Identifier:
1570272
Alternate Identifier(s):
OSTI ID: 1542691
Report Number(s):
SAND-2019-10359J
Journal ID: ISSN 0021-9606; 679028; TRN: US2001251
Grant/Contract Number:  
AC04-94AL85000; NA0003525
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 151; Journal Issue: 3; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN

Citation Formats

Jones, R. E., Tucker, W. C., Mills, M. J. L., and Mukerjee, S. Insight into hydrogen production through molecular simulation of an electrode-ionomer electrolyte system. United States: N. p., 2019. Web. doi:10.1063/1.5097609.
Jones, R. E., Tucker, W. C., Mills, M. J. L., & Mukerjee, S. Insight into hydrogen production through molecular simulation of an electrode-ionomer electrolyte system. United States. doi:https://doi.org/10.1063/1.5097609
Jones, R. E., Tucker, W. C., Mills, M. J. L., and Mukerjee, S. Sun . "Insight into hydrogen production through molecular simulation of an electrode-ionomer electrolyte system". United States. doi:https://doi.org/10.1063/1.5097609. https://www.osti.gov/servlets/purl/1570272.
@article{osti_1570272,
title = {Insight into hydrogen production through molecular simulation of an electrode-ionomer electrolyte system},
author = {Jones, R. E. and Tucker, W. C. and Mills, M. J. L. and Mukerjee, S.},
abstractNote = {In this work, we examine metal electrode-ionomer electrolyte systems at high voltage (negative surface charge) and at high pH to assess factors that influence hydrogen production efficiency. We simulate the hydrogen evolution electrode interface investigated experimentally in the work of Bates et al. [J. Phys. Chem. C 119, 5467 (2015)] using a combination of first principles calculations and classical molecular dynamics. With this detailed molecular information, we explore the hypotheses posed in the work of Bates et al. In particular, we examine the response of the system to increased bias voltage and oxide coverage in terms of the potential profile, changes in solvation and species concentrations away from the electrode, surface concentrations, and orientation of water at reactive surface sites. Finally, we discuss this response in the context of hydrogen production.},
doi = {10.1063/1.5097609},
journal = {Journal of Chemical Physics},
number = 3,
volume = 151,
place = {United States},
year = {2019},
month = {7}
}

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