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O: Fachverband Oberflächenphysik

O 18: Solid-Liquid Interfaces I: Structure and Spectroscopy

O 18.4: Talk

Monday, March 18, 2024, 15:45–16:00, H 1012

The Influence of Mesoscopic Surface Structure on the Electrocatalytic Selectivity of CO2 Reduction with UHV-Prepared Cu(111) Single Crystals — •Khanh-Ly Nguyen, Jared P. Bruce, Aram Yoon, Juan Navarro, Fabian Scholten, Felix Landwehr, Clara Rettenmaier, Markus Heyde, and Beatriz Roldan Cuenya — Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195 Berlin, Germany

Electrocatalytic conversion of CO2 to higher order hydrocarbons has been proposed as a promising approach to re-utilize the greenhouse CO2. The only pure metal that is capable of reducing CO2 to C2+ hydrocarbons is copper although it suffers from low selectivity. Cu(111) single crystal surfaces prepared under ultra-high vacuum (UHV) conditions were found to display different product selectivity during CO2RR despite similar chemical and local microscopic surface features. In particular, changes in selectivity from hydrogen-dominant to hydrocarbon-dominant product distributions were observed based on the number of CO2RR electrolysis and subsequent UHV treatments. 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 CO2RR and that not only atomistic but also mesoscale characterization of electrocatalytic materials is needed in order to comprehend complex selectivity trends.

Keywords: CO2 Reduction Reaction; Copper Single Crystal; SEM STM; Stepped Surfaces; Mesoscopic Structure