Chemical Pressure-Driven Enhancement of the Hydrogen Evolving Activity of Ni2P from Nonmetal Surface Doping Interpreted via Machine Learning

Wexler, Robert B.; Martirez, John Mark P.; Rappe, Andrew M.

doi:10.1021/jacs.8b00947

Chemical Pressure-Driven Enhancement of the Hydrogen Evolving Activity of Ni₂P from Nonmetal Surface Doping Interpreted via Machine Learning

Journal Article · Mon Mar 19 00:00:00 UTC 2018 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.8b00947· OSTI ID:1489143

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Univ. of Pennsylvania, Philadelphia, PA (United States). Dept. of Chemistry
Princeton Univ., Princeton, NJ (United States). Dept. of Mechanical and Aerospace Engineering

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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center

Sponsoring Organization:: USDOE

OSTI ID:: 1489143

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 13 Vol. 140; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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