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

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

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

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

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

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

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

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

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

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

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

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

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

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Monteiro,  Mariana C. O.       
Interface Science, Fritz Haber Institute, Max Planck Society;

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

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Zitation

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.


Zitierlink: https://hdl.handle.net/21.11116/0000-000F-47C4-4
Zusammenfassung
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.