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

Janis Timoshenko (), Clara Rettenmaier, Dorottya Hursán, Martina Rüscher, Eduardo Ortega, Antonia Herzog, Timon Wagner, Arno Bergmann, Uta Hejral, Aram Yoon, Andrea Martini, Eric Liberra, Mariana Cecilio de Oliveira Monteiro and Beatriz Roldan Cuenya ()
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Janis Timoshenko: Fritz-Haber Institute of the Max-Planck Society
Clara Rettenmaier: Fritz-Haber Institute of the Max-Planck Society
Dorottya Hursán: Fritz-Haber Institute of the Max-Planck Society
Martina Rüscher: Fritz-Haber Institute of the Max-Planck Society
Eduardo Ortega: Fritz-Haber Institute of the Max-Planck Society
Antonia Herzog: Fritz-Haber Institute of the Max-Planck Society
Timon Wagner: Fritz-Haber Institute of the Max-Planck Society
Arno Bergmann: Fritz-Haber Institute of the Max-Planck Society
Uta Hejral: Fritz-Haber Institute of the Max-Planck Society
Aram Yoon: Fritz-Haber Institute of the Max-Planck Society
Andrea Martini: Fritz-Haber Institute of the Max-Planck Society
Eric Liberra: Fritz-Haber Institute of the Max-Planck Society
Mariana Cecilio de Oliveira Monteiro: Fritz-Haber Institute of the Max-Planck Society
Beatriz Roldan Cuenya: Fritz-Haber Institute of the Max-Planck Society

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-50379-w

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