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 Cecilio de Oliveira, Cuenya Beatriz Roldan
Department of Interface Science, Fritz-Haber Institute of the Max-Planck Society, Berlin, Germany.
Nat Commun. 2024 Jul 20;15(1):6111. doi: 10.1038/s41467-024-50379-w.
Copper and nitrogen co-doped carbon catalysts exhibit a remarkable behavior during the electrocatalytic CO reduction (CORR), 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 CORR products, a lack of which has thus far hindered the wide-spread practical adoption of CORR. 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 CORR functionalities.
铜和氮共掺杂的碳催化剂在电催化CO还原（CORR）过程中表现出显著的行为，即从铜单原子形成金属纳米颗粒，以及随后它们的可逆再分散。在这里我们表明，这些物种的可切换性质是按需控制CORR产物分布的关键，而缺乏这种控制迄今为止阻碍了CORR的广泛实际应用。通过用阳极电势脉冲间歇工作阴极电势脉冲，我们能够实现铜颗粒的可控破碎和单原子位点的部分再生。通过调整脉冲持续时间，并使用原位快速X射线吸收光谱跟踪催化剂的演变，可以将催化剂的形态导向单原子位点、超小金属簇或大金属纳米颗粒，每种都表现出独特的CORR功能。
