Monolayer nitrides doped with transition metals as efficient catalysts for water oxidation: the singular role of nickel

Qiuhua Liang, Geert Brocks, Xueqing Zhang, Anja Bieberle-Hütter (Corresponding author)

Research output: Contribution to journalArticleAcademicpeer-review

Abstract

Exploration of precious-metal-free catalysts for water splitting is of great importance in developing renewable energy conversion and storage technologies. In this paper, on the basis of density functional theory calculations, we reveal the link between the oxygen evolution reaction (OER) activities and the electronic properties of pure and first-row transition-metal (TM)-doped AlN and GaN two-dimensional monolayers. We find that Ni-doped layers are singularly appealing because they lead to a low overpotential (0.4 V). Early TM dopants are not suited for the OER because they bind the intermediate species OH or O too strongly, which leads to very large overpotentials, or no OER activity at all. The late TM dopants Cu and Zn show less or no OER activity as they bind the intermediate species too weakly. Although in many cases the overpotential can be traced back to an OOH intermediate species being adsorbed too weakly compared to an OH species, the Ni dopant breaks this rule by stabilizing the OOH adsorbant. The stabilization can be correlated with a switch from a high-spin to a low-spin state of the dopant atom. This ability to change spin states offers an exciting ingredient for the design of OER catalysts.

Original languageEnglish
Pages (from-to)26289-26298
Number of pages10
JournalJournal of Physical Chemistry C
Volume123
Issue number43
DOIs
Publication statusPublished - 31 Oct 2019

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Nickel
Nitrides
Transition metals
nitrides
Monolayers
transition metals
nickel
Oxygen
catalysts
Oxidation
oxidation
Catalysts
Doping (additives)
Water
oxygen
water
water splitting
renewable energy
energy conversion
energy storage

Cite this

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title = "Monolayer nitrides doped with transition metals as efficient catalysts for water oxidation: the singular role of nickel",
abstract = "Exploration of precious-metal-free catalysts for water splitting is of great importance in developing renewable energy conversion and storage technologies. In this paper, on the basis of density functional theory calculations, we reveal the link between the oxygen evolution reaction (OER) activities and the electronic properties of pure and first-row transition-metal (TM)-doped AlN and GaN two-dimensional monolayers. We find that Ni-doped layers are singularly appealing because they lead to a low overpotential (0.4 V). Early TM dopants are not suited for the OER because they bind the intermediate species OH or O too strongly, which leads to very large overpotentials, or no OER activity at all. The late TM dopants Cu and Zn show less or no OER activity as they bind the intermediate species too weakly. Although in many cases the overpotential can be traced back to an OOH intermediate species being adsorbed too weakly compared to an OH species, the Ni dopant breaks this rule by stabilizing the OOH adsorbant. The stabilization can be correlated with a switch from a high-spin to a low-spin state of the dopant atom. This ability to change spin states offers an exciting ingredient for the design of OER catalysts.",
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Monolayer nitrides doped with transition metals as efficient catalysts for water oxidation : the singular role of nickel. / Liang, Qiuhua; Brocks, Geert; Zhang, Xueqing; Bieberle-Hütter, Anja (Corresponding author).

In: Journal of Physical Chemistry C, Vol. 123, No. 43, 31.10.2019, p. 26289-26298.

Research output: Contribution to journalArticleAcademicpeer-review

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