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Superiority of the (100) Over the (111) Facets of the Nitrides for Hydrogen Evolution Reaction

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Abstract

In continuation of our previous DFT calculations on the possibility of using the earlier transition metal nitrides for catalyzing hydrogen evolution reaction, this work analyzes the (111) facets of these surfaces which are as dominant as the (100) when a polycrystalline catalyst is manufactured. Various hydrogen coverage on these surfaces is considered, the free energy diagram and overpotentials are predicted as well as the kinetics of hydrogen recombination and hydrogen evolution reaction. The outcome of this comprehensive investigation and comparison of activity between the (100) and (111) facets reveal that TaN is the most active surface in both facets with the (100) being more promising with regards to both thermodynamics and kinetics. This study suggests that for optimizing the efficiency in the experiments, surface engineering needs to be considered towards the synthesis of single-crystal structured catalysts rather than utilizing polycrystallines. All the results are also compared with the Pt (111) which is the most active hydrogen evolution catalyst.

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Fig. 1

taken from ref [25] and is shown with dashed line. The studied (111) surfaces are shown with solid lines

Fig. 2
Fig. 3

adapted from ref [25]

Fig. 4

adapted from ref [25]. In order to reach 2/8 coverage of H on TaN, − 0.45 V needs to be applied and this naturally results in more H coverage, thus some of the points are overlaying at − 0.45 V for TaN

Fig. 5

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Data Availability

The datasets generated during and/or analysed during the current study are available from the corresponding author on reasonable request.

Code Availability

The VASP code was used for the DFT calculations of this manuscript and the corresponding details of that are provided in the manuscript.

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Acknowledgements

Financial support is acknowledged from the Icelandic Research Fund grant numbers 185051051-3, 207056-051, 207056-052, and the Research Fund of the University of Iceland. The calculations were carried out on the Icelandic high-performance computer, Garpur.

Funding

Icelandic research Fund grant numbers 185051051-3, 207056-051, 207056-052, and the Research Fund of the University of Iceland.

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    Younes Abghoui

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Abghoui, Y. Superiority of the (100) Over the (111) Facets of the Nitrides for Hydrogen Evolution Reaction. Top Catal 65, 262–269 (2022). https://doi.org/10.1007/s11244-021-01474-5

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