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Computational high-throughput screening of electrocatalytic materials for hydrogen evolution

Nature Materials volume 5, pages 909–913 (2006)Cite this article

Abstract

The pace of materials discovery for heterogeneous catalysts and electrocatalysts could, in principle, be accelerated by the development of efficient computational screening methods. This would require an integrated approach, where the catalytic activity and stability of new materials are evaluated and where predictions are benchmarked by careful synthesis and experimental tests. In this contribution, we present a density functional theory-based, high-throughput screening scheme that successfully uses these strategies to identify a new electrocatalyst for the hydrogen evolution reaction (HER). The activity of over 700 binary surface alloys is evaluated theoretically; the stability of each alloy in electrochemical environments is also estimated. BiPt is found to have a predicted activity comparable to, or even better than, pure Pt, the archetypical HER catalyst. This alloy is synthesized and tested experimentally and shows improved HER performance compared with pure Pt, in agreement with the computational screening results.

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Figure 1: Volcano plot for the HER for various pure metals and metal overlayers.
Figure 2: Schematic diagrams of surface alloys at the solute coverages for which calculations are carried out.
Figure 3: Computational high-throughput screening for |ΔGH| on 256 pure metals and surface alloys.
Figure 4: Pareto-optimal plot of stability and activity of surface alloys for the HER.
Figure 5: Hydrogen evolution after each stage of BiPt surface alloy synthesis on a fluorine-doped tin-oxide substrate.

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Acknowledgements

J.G. and T.F.J. acknowledge H. C. Ørsted Postdoctoral Fellowships from the Technical University of Denmark. J.B. acknowledges support from the Danish Strategic Research Council. The Center for Individual Nanoparticle Functionality is supported by the Danish National Research Foundation. The Center for Atomic-scale Materials Design is supported by the Lundbeck Foundation. We thank the Danish Center for Scientific Computing for computer time. We also thank K. P. Jørgensen and J. Larsen for technical assistance.

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Authors and Affiliations

  1. Department of Physics, Center for Atomic-scale Materials Design, NanoDTU, Technical Univ. of Denmark, DK-2800, Kongens Lyngby, Denmark

    Jeff Greeley & Jens K. Nørskov

  2. Department of Physics, Center for Individual Nanoparticle Functionality, NanoDTU, Technical Univ. of Denmark, DK-2800, Kongens Lyngby, Denmark

    Thomas F. Jaramillo, Jacob Bonde & Ib Chorkendorff

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  1. Jeff Greeley
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Correspondence to Jens K. Nørskov.

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Greeley, J., Jaramillo, T., Bonde, J. et al. Computational high-throughput screening of electrocatalytic materials for hydrogen evolution. Nature Mater 5, 909–913 (2006). https://doi.org/10.1038/nmat1752

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