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Trends in reactivity of electrodeposited 3d transition metals on gold revealed by operando soft x-ray absorption spectroscopy during water splitting

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Velasco Vélez,  Juan
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Department of Heterogeneous Reactions, Max Planck Institute for Chemical Energy Conversion;

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Jones,  Travis
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Pfeifer,  Verena
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Schlögl,  Robert
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Department of Heterogeneous Reactions, Max Planck Institute for Chemical Energy Conversion;

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Zitation

Velasco Vélez, J., Jones, T., Pfeifer, V., Dong, C.-L., Chen, Y.-X., Chen, C.-M., et al. (2017). Trends in reactivity of electrodeposited 3d transition metals on gold revealed by operando soft x-ray absorption spectroscopy during water splitting. Journal of Physics D, 50(2): 024002. doi:10.1088/1361-6463/50/2/024002.


Zitierlink: http://hdl.handle.net/11858/00-001M-0000-002C-1B5D-1
Zusammenfassung
We activated gold electrodes for their use as electrocatalyst for water splitting by electrodepositing Cu, Ni and Co. A combination of operando x-ray absorption spectroscopy and potentiometric control under aqueous conditions revealed the trends in reactivity yielded by these electrodes, which are directly associated with the cross- and overpotentials as well as the occupancy of the 3d orbitals. It was found that under anodic polarization the materials electrodeposited on gold suffer from a lack of stability, while under cathodic polarization they exhibit stable behavior. The observed activity is strongly related to the lack of stability shown by these composites under anodic polarization revealing a dynamic process ruled by corrosion. By operando x-ray absorption, we established that the overall enhancement of the activity for the oxygen evolution reaction is directly attributable to the cross-potential and corrosion process of the electrodeposited materials. It is associated with the high potential deposition, which is the origin of the incipient oxidation-corrosion resistance of the lattice. We conclude that the observed trends in the total current are directly associated with the loss of oxygen in the metal-oxide lattice and the subsequent dissolution of metallic ions in the electrolyte under anodic polarization.