Steering the structure and selectivity of CO2 electroreduction catalysts by 
potential pulses

Timoshenko, Janis; Bergmann, Arno; Rettenmaier, Clara; Herzog, Antonia; Aran Ais, Rosa; Jeon, Hyosang; Haase, Felix; Hejral, Uta; Grosse, Philipp; Kühl, Stefanie; Davis, Earl; Tian, Jing; Magnussen, Olaf; Roldan Cuenya, Beatriz

doi:10.1038/s41929-022-00760-z

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Steering the structure and selectivity of CO₂ electroreduction catalysts by potential pulses

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

/persons/resource/persons214068

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

/persons/resource/persons227610

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

/persons/resource/persons232519

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

/persons/resource/persons227595

Aran Ais, Rosa
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons227603

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

/persons/resource/persons227601

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

/persons/resource/persons75574

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

/persons/resource/persons227599

Grosse, Philipp
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons21771

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

/persons/resource/persons126961

Davis, Earl
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

Timoshenko, J., Bergmann, A., Rettenmaier, C., Herzog, A., Aran Ais, R., Jeon, H., et al. (2022). Steering the structure and selectivity of CO₂ electroreduction catalysts by potential pulses. Nature Catalysis, 5(4), 259-267. doi:10.1038/s41929-022-00760-z.

Cite as: https://hdl.handle.net/21.11116/0000-0009-F9C3-2

Abstract

Convoluted selectivity trends and a missing link between reaction product distribution and catalyst properties hinder practical applications of the electrochemical CO₂ reduction reaction (CO₂RR) for multicarbon product generation. Here we employ operando X-ray absorption and X-ray diffraction methods with subsecond time resolution to unveil the surprising complexity of catalysts exposed to dynamic reaction conditions. We show that by using a pulsed reaction protocol consisting of alternating working and oxidizing potential periods that dynamically perturb catalysts derived from Cu₂O nanocubes, one can decouple the effect of the ensemble of coexisting copper species on the product distribution. In particular, an optimized dynamic balance between oxidized and reduced copper surface species achieved within a narrow range of cathodic and anodic pulse durations resulted in a twofold increase in ethanol production compared with static CO₂RR conditions. This work thus prepares the ground for steering catalyst selectivity through dynamically controlled structural and chemical transformations.