Time-resolved operando insights into the tunable selectivity of Cu–Zn nanocubes 
during pulsed CO2 electroreduction

Herzog, Antonia; Rüscher, Martina; Jeon, Hyosang; Timoshenko, Janis; Rettenmaier, Clara; Hejral, Uta; Davis, Earl; Haase, Felix; Kordus, David; Kühl, Stefanie; Frandsen, Wiebke; Bergmann, Arno; Roldan Cuenya, Beatriz

doi:10.1039/D4EE02308K

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Time-resolved operando insights into the tunable selectivity of Cu–Zn nanocubes during pulsed CO₂ electroreduction

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/persons/resource/persons232519

Herzog, Antonia
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons267176

Rüscher, Martina
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons227603

Jeon, Hyosang
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons227619

Timoshenko, Janis
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons227610

Rettenmaier, Clara
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons75574

Hejral, Uta
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons126961

Davis, Earl
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons227601

Haase, Felix
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons227605

Kordus, David
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons21771

Kühl, Stefanie
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons21518

Frandsen, Wiebke
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons214068

Bergmann, Arno
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons22020

Roldan Cuenya, Beatriz
Interface Science, Fritz Haber Institute, Max Planck Society;

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Citation

Herzog, A., Rüscher, M., Jeon, H., Timoshenko, J., Rettenmaier, C., Hejral, U., et al. (2024). Time-resolved operando insights into the tunable selectivity of Cu–Zn nanocubes during pulsed CO₂ electroreduction. Energy & Environmental Science, 17(19), 7081-7096. doi:10.1039/D4EE02308K.

Cite as: https://hdl.handle.net/21.11116/0000-000F-C427-8

Abstract

Pulsed electrochemical CO₂ reduction (CO₂RR) has emerged as a facile way to alter the product selectivities toward desired multicarbon products, but so far, it has been mainly applied to monometallic Cu-based electrodes, which suffer from stability issues. Here, ZnO-decorated Cu₂O nanocubes were exposed to various pulsed CO₂RR treatments to uncover the effect of the redox transitions of both metals on the dynamic catalyst structure and composition and its link to their catalytic function. Here, an increase in the ethanol selectivity was observed once pulsed into the oxidation regime of zinc, while the parasitic hydrogen evolution drastically increased once pulsed into the oxidation regime of Cu. By employing time-resolved operando X-ray absorption spectroscopy, X-ray diffraction, and surface-enhanced Raman spectroscopy, we could follow the dynamically induced interplay between Zn oxide, CuZn alloy, metallic Zn and metallic Cu formation, and the coverage of co-adsorbed hydroxide and *CO. Our study highlights the relevance of zinc oxide and an increased OH coverage for the enhancement of the catalyst selectivity toward ethanol.