The Influence of Mesoscopic Surface Structure on the Electrocatalytic Selectivity of CO 2 Reduction with UHV-Prepared Cu(111) Single Crystals.

Autor: Nguyen KC; Department of Interface Science, Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, Berlin 14195, Germany., Bruce JP; Department of Interface Science, Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, Berlin 14195, Germany., Yoon A; Department of Interface Science, Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, Berlin 14195, Germany., Navarro JJ; Department of Interface Science, Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, Berlin 14195, Germany., Scholten F; Department of Interface Science, Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, Berlin 14195, Germany., Landwehr F; Department of Interface Science, Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, Berlin 14195, Germany., Rettenmaier C; Department of Interface Science, Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, Berlin 14195, Germany., Heyde M; Department of Interface Science, Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, Berlin 14195, Germany., Cuenya BR; Department of Interface Science, Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, Berlin 14195, Germany.
Jazyk: angličtina
Zdroj: ACS energy letters [ACS Energy Lett] 2024 Jan 29; Vol. 9 (2), pp. 644-652. Date of Electronic Publication: 2024 Jan 29 (Print Publication: 2024).
DOI: 10.1021/acsenergylett.3c02693
Abstrakt: The key role of morphological defects (e.g., irregular steps and dislocations) on the selectivity of model Cu catalysts for the electrocatalytic reduction of CO 2 (CO 2 RR) is illustrated here. Cu(111) single-crystal surfaces prepared under ultrahigh vacuum (UHV) conditions and presenting similar chemical and local microscopic surface features were found to display different product selectivity during the CO 2 RR. In particular, changes in selectivity from hydrogen-dominant to hydrocarbon-dominant product distributions were observed based on the number of CO 2 RR electrolysis pretreatment cycles performed prior to a subsequent UHV surface regeneration treatment, which lead to surfaces with seemingly identical chemical composition and local crystallographic structure. However, significant mesostructural changes were observed through a micron-scale microscopic analysis, including a higher density of irregular steps on the samples producing hydrocarbons. Thus, our findings highlight that step edges are key for C-C coupling in the CO 2 RR and that not only atomistic but also mesoscale characterization of electrocatalytic materials is needed in order to comprehend complex selectivity trends.
Competing Interests: The authors declare no competing financial interest.
(© 2024 The Authors. Published by American Chemical Society.)
Databáze: MEDLINE
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