Chemical Pressure-Driven Enhancement of the Hydrogen Evolving Activity of Ni2P from Nonmetal Surface Doping Interpreted via Machine Learning
Abstract
The activity of Ni2P catalysts for the hydrogen evolution reaction (HER) is currently limited by strong H adsorption at the Ni3-hollow site. We investigate the effect of surface nonmetal doping on the HER activity of the Ni3P2 termination of Ni2P(0001), which is stable at modest electrochemical conditions. Using density functional theory (DFT) calculations, we find that both 2p nonmetals and heavier chalcogens provide nearly thermoneutral H adsorption at moderate surface doping concentrations. We also find, however, that only chalcogen substitution for surface P is exergonic. For intermediate surface concentrations of S, the free energy of H adsorption at the Ni3-hollow site is -0.11 eV, which is significantly more thermoneutral than the undoped surface (-0.45 eV). We use the regularized random forest machine learning algorithm to discover the relative importance of structure and charge descriptors, extracted from the DFT calculations, in determining the HER activity of Ni2P(0001) under different doping concentrations. Here, we discover that the Ni–Ni bond length is the most important descriptor of HER activity, which suggests that the nonmetal dopants induce a chemical pressure-like effect on the Ni3-hollow site, changing its reactivity through compression and expansion.
- Authors:
-
[1];
[2];
[1]
- Univ. of Pennsylvania, Philadelphia, PA (United States). Dept. of Chemistry
- Princeton Univ., Princeton, NJ (United States). Dept. of Mechanical and Aerospace Engineering
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1489143
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 140; Journal Issue: 13; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Wexler, Robert B., Martirez, John Mark P., and Rappe, Andrew M. Chemical Pressure-Driven Enhancement of the Hydrogen Evolving Activity of Ni2P from Nonmetal Surface Doping Interpreted via Machine Learning. United States: N. p., 2018.
Web. doi:10.1021/jacs.8b00947.
Wexler, Robert B., Martirez, John Mark P., & Rappe, Andrew M. Chemical Pressure-Driven Enhancement of the Hydrogen Evolving Activity of Ni2P from Nonmetal Surface Doping Interpreted via Machine Learning. United States. https://doi.org/10.1021/jacs.8b00947
Wexler, Robert B., Martirez, John Mark P., and Rappe, Andrew M. Mon .
"Chemical Pressure-Driven Enhancement of the Hydrogen Evolving Activity of Ni2P from Nonmetal Surface Doping Interpreted via Machine Learning". United States. https://doi.org/10.1021/jacs.8b00947. https://www.osti.gov/servlets/purl/1489143.
@article{osti_1489143,
title = {Chemical Pressure-Driven Enhancement of the Hydrogen Evolving Activity of Ni2P from Nonmetal Surface Doping Interpreted via Machine Learning},
author = {Wexler, Robert B. and Martirez, John Mark P. and Rappe, Andrew M.},
abstractNote = {The activity of Ni2P catalysts for the hydrogen evolution reaction (HER) is currently limited by strong H adsorption at the Ni3-hollow site. We investigate the effect of surface nonmetal doping on the HER activity of the Ni3P2 termination of Ni2P(0001), which is stable at modest electrochemical conditions. Using density functional theory (DFT) calculations, we find that both 2p nonmetals and heavier chalcogens provide nearly thermoneutral H adsorption at moderate surface doping concentrations. We also find, however, that only chalcogen substitution for surface P is exergonic. For intermediate surface concentrations of S, the free energy of H adsorption at the Ni3-hollow site is -0.11 eV, which is significantly more thermoneutral than the undoped surface (-0.45 eV). We use the regularized random forest machine learning algorithm to discover the relative importance of structure and charge descriptors, extracted from the DFT calculations, in determining the HER activity of Ni2P(0001) under different doping concentrations. Here, we discover that the Ni–Ni bond length is the most important descriptor of HER activity, which suggests that the nonmetal dopants induce a chemical pressure-like effect on the Ni3-hollow site, changing its reactivity through compression and expansion.},
doi = {10.1021/jacs.8b00947},
journal = {Journal of the American Chemical Society},
number = 13,
volume = 140,
place = {United States},
year = {Mon Mar 19 00:00:00 EDT 2018},
month = {Mon Mar 19 00:00:00 EDT 2018}
}
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