Dynamic Changes in the Structure, Chemical State and Catalytic Selectivity of 
Cu Nanocubes during CO2 Electroreduction: Size and Support Effects

Grosse, Philipp; Gao, Dunfeng; Scholtenn, Fabian; Sinev, Ilya; Mistry, Hemma; Roldan Cuenya, Beatriz

doi:10.1002/anie.201802083

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Dynamic Changes in the Structure, Chemical State and Catalytic Selectivity of Cu Nanocubes during CO₂ Electroreduction: Size and Support Effects

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Roldan Cuenya, Beatriz
Department of Physics, University of Central Florida;
Interface Science, Fritz Haber Institute, Max Planck Society;
Department of Physics, Ruhr-University Bochum, 44780 Bochum, Germany;

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引用

Grosse, P., Gao, D., Scholtenn, F., Sinev, I., Mistry, H., & Roldan Cuenya, B. (2018). Dynamic Changes in the Structure, Chemical State and Catalytic Selectivity of Cu Nanocubes during CO₂ Electroreduction: Size and Support Effects. Angewandte Chemie International Edition, 57(21), 6192-6197. doi:10.1002/anie.201802083.

引用: https://hdl.handle.net/21.11116/0000-0001-2364-7

要旨

In situ and operando spectroscopic and microscopic methods were used to gain insight into the correlation between the structure, chemical state, and reactivity of size‐ and shape‐controlled ligand‐free Cu nanocubes (Cu‐cubes) during CO₂ electroreduction (CO₂RR). Dynamic changes in the morphology and composition of Cu‐cubes supported on carbon were monitored under potential control via electrochemical atomic force microscopy, X‐ray absorption fine‐structure spectroscopy and X‐ray photoelectron spectroscopy. Under reaction conditions, the roughening of the nanocube surface, disappearance of the (100) facets, formation of pores, loss of Cu and reduction of CuO_x species observed were found to lead to a suppression of the selectivity for multi‐carbon products (i.e. C₂H₄ and ethanol) versus CH₄. A comparison with Cu‐cubes supported on Cu foils revealed an enhanced morphological stability and persistence of Cu(I) species under CO₂RR. Both factors are held responsible for the higher C₂/C₁ product ratio observed for the Cu cubes/Cu as compared to Cu cubes/C. Our findings highlight the importance of the structure of the active nanocatalyst but also its interaction with the underlying substrate in CO₂RR selectivity.