Catalysts for Hydrogen Evolution from the [NiFe] Hydrogenase to the Ni 2 P(001) Surface: The Importance of Ensemble Effect

Liu, Ping; Rodriguez, José A.

doi:10.1021/ja0540019

Cited by 1,240Electrocatalysts for Energy ConversionMetalloenzymes and iron-sulfur proteinsCO2 Reduction Techniques and Catalysts

Catalysts for Hydrogen Evolution from the [NiFe] Hydrogenase to the Ni 2 P(001) Surface: The Importance of Ensemble Effect

Liu, Ping, Rodriguez, José A.·2005·Journal of the American Chemical Society

DOI 10.1021/ja0540019

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Abstract

Density functional theory (DFT) was employed to investigate the behavior of a series of catalysts used in the hydrogen evolution reaction (HER, 2H(+) + 2e(-) --> H(2)). The kinetics of the HER was studied on the [NiFe] hydrogenase, the [Ni(PS3*)(CO)](1)(-) and [Ni(PNP)(2)](2+) complexes, and surfaces such as Ni(111), Pt(111), or Ni(2)P(001). Our results show that the [NiFe] hydrogenase exhibits the highest activity toward the HER, followed by [Ni(PNP)(2)](2+) > Ni(2)P > [Ni(PS3*)(CO)](1)(-) > Pt > Ni in a decreasing sequence. The slow kinetics of the HER on the surfaces is due to the fact that the metal hollow sites bond hydrogen too strongly to allow the facile removal of H(2). In fact, the strong H-Ni interaction on Ni(2)P(001) can lead to poisoning of the highly active sites of the surface, which enhances the rate of the HER and makes it comparable to that of the [NiFe] hydrogenase. In contrast, the promotional effect of H-poisoning on the HER on Pt and Ni surfaces is relatively small. Our calculations suggest that among all of the systems investigated, Ni(2)P should be the best practical catalyst for the HER, combining the high thermostability of the surfaces and high catalytic activity of the [NiFe] hydrogenase. The good behavior of Ni(2)P(001) toward the HER is found to be associated with an ensemble effect, where the number of active Ni sites is decreased due to presence of P, which leads to moderate bonding of the intermediates and products with the surface. In additi…

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Previous reports have demonstrated the crucial roles of transition metal phosphides for HER by density functional theory calculations.
“Previous reports have been demonstrated the crucial roles of TMPs for HER by density functional theory (DFT) calculations [74,75].”
From Ultrathin nickel phosphide nanosheet aerogel electrocatalysts derived from Ni-alginate for hydrogen evolution reaction (2020) · cites this paper as [74]
P atoms in transition metal phosphides play crucial roles, with negatively charged P acting as a base to trap positively charged protons during electrochemical HER.
“It has been proven that P atoms in TMPs play crucial roles, in that the negatively charged P acts as a base to trap positively charged protons during electrochemical HER.45,46”
From M X P(M = Co/Ni)@carbon core–shell nanoparticles embedded in 3D cross-linked graphene aerogel derived from seaweed biomass for hydrogen evolution reaction (2018) · cites this paper as [45]

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Authors: Liu, P., & Rodriguez, J. A.
Affiliations: Brookhaven National Laboratory (US)
Contribution from the Department of Chemistry, Brookhaven National Laboratory, Building 555, Upton, New York 11973
ORCID: Liu, Ping
Venue: Journal of the American Chemical Society
Publisher: American Chemical Society (ACS)
Published: 2005-10-01
Volume: 127
Issue: 42
Pages: 14871-14878
ISSN: 0002-7863 (ISSN-L)
1520-5126
DOI: 10.1021/ja0540019
OpenAlex: W1996802576
Cited by: 1,240
References: 40
Citations by year: 2026: 60 · 2025: 85 · 2024: 93 · 2023: 103 · 2022: 132 · 2021: 131 · 2020: 122 · 2019: 133 · 2018: 113 · 2017: 73 · 2016: 67 · 2015: 47 · 2014: 44 · 2013: 9 · 2012: 5
FWCI: 4.50
Type: journal article
Language: en
Open access: closed
Locations: Journal of the American Chemical Society (publishedVersion)
PubMed (publishedVersion)
Topics: Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Metalloenzymes and iron-sulfur proteins
Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
Keywords: hydrogen evolution reaction, [NiFe] hydrogenase, Pt(111), Ni(111) surface, hydrogen poisoning, ensemble effect, catalytic activity, hydrogenase mimics, phosphine ligands
MeSH terms: Catalysis, Hydrogen, Hydrogenase, Kinetics, Models, Chemical, Nickel, Organometallic Compounds, Surface Properties

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Catalysts for Hydrogen Evolution from the [NiFe] Hydrogenase to the Ni 2 P(001) Surface: The Importance of Ensemble Effect

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