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Rational strain engineering in delafossite oxides for highly efficient hydrogen evolution catalysis in acidic media

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Zhang,  Siyuan
Nanoanalytics and Interfaces, Independent Max Planck Research Groups, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Diehl,  Leo
Max Planck Institute for Solid State Research, Max Planck Society;
Department of Chemistry, Ludwig Maximilian University of Munich, Munich, Germany;

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Duppel,  Viola
Max Planck Institute for Solid State Research, Max Planck Society;

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Richter,  Gunther
Central Scientific Facility Materials, Max Planck Institute for Intelligent Systems, Max Planck Society;

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Scheu,  Christina
Nanoanalytics and Interfaces, Independent Max Planck Research Groups, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Citation

Podjaski, F., Weber, D., Zhang, S., Diehl, L., Eger, R., Duppel, V., et al. (2020). Rational strain engineering in delafossite oxides for highly efficient hydrogen evolution catalysis in acidic media. Nature Catalysis, 3(1), 55-63. doi:10.1038/s41929-019-0400-x.


Cite as: http://hdl.handle.net/21.11116/0000-0009-2E58-2
Abstract
The rational design of hydrogen evolution reaction electrocatalysts that can compete with platinum is an outstanding challenge in the process of designing viable power-to-gas technologies. Here, we introduce delafossites as a family of hydrogen evolution reaction electrocatalysts in acidic media. We show that, in PdCoO2, the inherently strained Pd metal sublattice acts as a pseudomorphic template for the growth of a tensile-strained Pd-rich capping layer under reductive conditions. The surface modification ranges up to 400 nm and continuously improves the electrocatalytic activity by simultaneously increasing the exchange current density and by reducing the Tafel slope down to 38 mV dec−1, leading to overpotentials η10 lt; 15 mV. The improved activity is attributed to the operando stabilization of a β-PdHx phase with enhanced surface catalytic properties with respect to pure or nanostructured palladium. These findings illustrate how operando-induced electrodissolution can be used as a top-down design concept through the strain-stabilized formation of catalytically active phases. © 2019, The Author(s), under exclusive licence to Springer Nature Limited.