The DOI matches its Crossref record; 18 of the 18 references it cites were found in a registry or an index.
Climbing the Volcano of Electrocatalytic Activity while Avoiding Catalyst Corrosion: Ni3P, a Hydrogen Evolution Electrocatalyst Stable in Both Acid and Alkali
Abstract
We report microcrystalline Ni 3 P as a noble-metal-free electrocatalyst for the H 2 evolution reaction (HER) with high activity just below those of Ni 5 P 4 and Pt, the two most efficient HER catalysts known. Ni 3 P has previously been dismissed for the HER, owing to its anticipated corrosion and its low activity when formed as an impurity in amorphous alloys. We observe higher activity of single-phase Ni 3 P crystallites than for other nickel phosphides (except Ni 5 P 4 ) in acid, high corrosion tolerance in acid, and zero corrosion in alkali. We compare its electrocatalytic performance, corrosion stability, and intrinsic turnover rate to those of different transition-metal phosphides. Electrochemical studies reveal that poisoning of surface Ni sites does not block the HER, indicating P as the active site. Using density functional theory (DFT), we analyze the thermodynamic stability of Ni 3 P and compare it to experiments. DFT calculations predict that surface reconstruction of Ni 3 P (001) strongly favors P enrichment of the Ni 4 P 4 termination and that the H adsorption energy depends strongly on the surface reconstruction, thus revealing a potential synthetic lever for tuning HER catalytic activity. A particular P-enriched reconstructed surface on Ni 3 P(001) is predicted to be the most stable surface termination at intermediate P content, as well as providing the most active surface site at low overpotentials. The P adatoms present on this reconstructed surface are more active for HER at low overpotentials in comparison to any of the sites investigated on other terminations of Ni 3 P(001), as they possess nearly thermoneutral H adsorption. To our knowledge this is the first time reconstructed surfaces of transition-metal phosphides have been identified as having the most active surface site, with such good agreement with the experimentally observed catalytic current onset and Tafel slope. The active site geometry achieved through reconstruction identified in this work shows great similarity to that reported for Ni 2 P(0001) and Ni 5 P 4 (0001) facets, serving as a general design principle for the future development of even more active transition-metal phosphide catalysts and further climbing the volcano plot.
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Citations
Cites
Identification of Active Edge Sites for Electrochemical H 2 Evolution from MoS 2 Nanocatalysts
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MoS 2 Nanoparticles Grown on Graphene: An Advanced Catalyst for the Hydrogen Evolution Reaction
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Self-citationBiomimetic Hydrogen Evolution: MoS 2 Nanoparticles as Catalyst for Hydrogen Evolution
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Nanostructured Nickel Phosphide as an Electrocatalyst for the Hydrogen Evolution Reaction
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Hydrogen Oxidation and Evolution Reaction Kinetics on Platinum: Acid vs Alkaline Electrolytes
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An efficient and pH-universal ruthenium-based catalyst for the hydrogen evolution reaction
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Self-citationSkúlason, E., Tripkovic, V., Björketun, M. E., Gudmundsdóttir, S., Karlberg, G., Rossmeisl, J., Bligaard, T., Jónsson, H., & Nørskov, J. K. (2010) · The Journal of Physical Chemistry C · doi:10.1021/jp1048887 · Cited by 1,271
Highly Active Electrocatalysis of the Hydrogen Evolution Reaction by Cobalt Phosphide Nanoparticles
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Density Functional Theory for Electrocatalysis
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Nickel phosphide polymorphs with an active (001) surface as excellent catalysts for water splitting
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Metadata
- Authors
- Laursen, A. B., Wexler, R. B., Whitaker, M. J., Izett, E. J., Calvinho, K. U. D., Hwang, S., Rucker, R., Wang, H., Li, J., Garfunkel, E., Greenblatt, M., Rappe, A. M., & Dismukes, G. C.
- Venue
- ACS Catalysis
- Publisher
- American Chemical Society (ACS)
- Published
- 2018-04-03
- Volume
- 8
- Issue
- 5
- Pages
- 4408-4419
- ISSN
- 2155-5435 (ISSN-L)
- OpenAlex
- W2795606616
- Cited by
- 233
- References
- 18
- FWCI
- 5.83
- Type
- journal article
- Language
- en
- Open access
- closed
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