Searching novel complex solid solution electrocatalysts in unconventional element combinations

Olga A. Krysiak; Simon Schumacher; Alan Savan; Wolfgang Schuhmann; Alfred Ludwig; Corina Andronescu

doi:10.1007/s12274-021-3637-z

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Research Article | Open Access

Searching novel complex solid solution electrocatalysts in unconventional element combinations

Olga A. Krysiak^{¹^,^§}, Simon Schumacher^{²^,³^,^§}, Alan Savan^⁴, Wolfgang Schuhmann^¹(), Alfred Ludwig^{⁴^,⁵}(), Corina Andronescu^{²^,³}()

1 Analytical Chemistry–Center for Electrochemical Sciences (CES), Faculty of Chemistry and Biochemistry, Ruhr University Bochum, Universitätsstr. 150, D-44780 Bochum, Germany

2 Chemical Technology III, Faculty of Chemistry, Carl-Benz-Straße 199, D-47057 Duisburg, Germany

3 CENIDE - Center for Nanointegration University Duisburg Essen, Carl-Benz-Straße 199, D-47057 Duisburg, Germany

4 Chair for Materials Discovery and Interfaces, Institute for Materials, Faculty of Mechanical Engineering, Ruhr University Bochum, Universitätsstr. 150, D-44780 Bochum, Germany

5 ZGH, Ruhr University Bochum, Universitätsstr. 150, D-44780 Bochum, Germany

^§ Olga A. Krysiak and Simon Schumacher contributed equally to this work.

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Reliable high-throughput discovery strategy for complex solid solution electrocatalysts with unusual elemental compositions for the hydrogen evolution reaction and the oxygen reduction reaction is reported.

Abstract

Despite outstanding accomplishments in catalyst discovery, finding new, more efficient, environmentally neutral, and noble metal-free catalysts remains challenging and unsolved. Recently, complex solid solutions consisting of at least five different elements and often named as high-entropy alloys have emerged as a new class of electrocatalysts for a variety of reactions. The multicomponent combinations of elements facilitate tuning of active sites and catalytic properties. Predicting optimal catalyst composition remains difficult, making testing of a very high number of them indispensable. We present the high-throughput screening of the electrochemical activity of thin film material libraries prepared by combinatorial co-sputtering of metals which are commonly used in catalysis (Pd, Cu, Ni) combined with metals which are not commonly used in catalysis (Ti, Hf, Zr). Introducing unusual elements in the search space allows discovery of catalytic activity for hitherto unknown compositions. Material libraries with very similar composition spreads can show different activities vs. composition trends for different reactions. In order to address the inherent challenge of the huge combinatorial material space and the inability to predict active electrocatalyst compositions, we developed a high-throughput process based on co-sputtered material libraries, and performed high-throughput characterization using energy dispersive X-ray spectroscopy (EDS), scanning transmission electron microscopy (SEM), X-ray diffraction (XRD) and conductivity measurements followed by electrochemical screening by means of a scanning droplet cell. The results show surprising material compositions with increased activity for the oxygen reduction reaction and the hydrogen evolution reaction. Such data are important input data for future data-driven materials prediction.

Keywords

high-entropy alloys electrocatalysis high-throughput screening thin films hydrogen evolution reaction oxygen reduction reaction

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References

Yeh, J. W.; Chen, Y. L.; Lin, S. J.; Chen, S. K. High-entropy alloys—A new era of exploitation. MSF 2007, 560, 1–9.