Reversible metal cluster formation on Nitrogen-doped carbon controlling 
electrocatalyst particle size with subnanometer accuracy

Timoshenko, Janis; Rettenmaier, Clara; Hursán, Dorottya; Rüscher, Martina; Ortega, Eduardo; Herzog, Antonia; Wagner, Timon; Bergmann, Arno; Hejral, Uta; Yoon, Aram; Martini, Andrea; Liberra, Eric; Monteiro, Mariana C. O.; Roldan Cuenya, Beatriz

doi:10.1038/s41467-024-50379-w

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Reversible metal cluster formation on Nitrogen-doped carbon controlling electrocatalyst particle size with subnanometer accuracy

MPS-Authors

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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/persons291371

Hursán, Dorottya
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons267176

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

/persons/resource/persons291374

Ortega, Eduardo
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons232519

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

/persons/resource/persons298330

Wagner, Timon
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons214068

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

/persons/resource/persons75574

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

/persons/resource/persons244720

Yoon, Aram
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons291369

Martini, Andrea
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons298334

Liberra, Eric
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons296152

Monteiro, Mariana C. O.
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., Rettenmaier, C., Hursán, D., Rüscher, M., Ortega, E., Herzog, A., et al. (2024). Reversible metal cluster formation on Nitrogen-doped carbon controlling electrocatalyst particle size with subnanometer accuracy. Nature Communications, 15: 6111. doi:10.1038/s41467-024-50379-w.

Cite as: https://hdl.handle.net/21.11116/0000-000F-47C4-4

Abstract

Copper and nitrogen co-doped carbon catalysts exhibit a remarkable behavior during the electrocatalytic CO₂ reduction (CO2RR), namely, the formation of metal nanoparticles from Cu single atoms, and their subsequent reversible redispersion. Here we show that the switchable nature of these species holds the key for the on-demand control over the distribution of CO₂RR products, a lack of which has thus far hindered the wide-spread practical adoption of CO₂RR. By intermitting pulses of a working cathodic potential with pulses of anodic potential, we were able to achieve a controlled fragmentation of the Cu particles and partial regeneration of single atom sites. By tuning the pulse durations, and by tracking the catalyst’s evolution using operando quick X-ray absorption spectroscopy, the speciation of the catalyst can be steered toward single atom sites, ultrasmall metal clusters or large metal nanoparticles, each exhibiting unique CO₂RR functionalities.