English
 
Help Privacy Policy Disclaimer
  Advanced SearchBrowse

Item

ITEM ACTIONSEXPORT

Released

Journal Article

Identifying structure-selectivity correlations in the electrochemical reduction of CO2: a comparison of well-ordered atomically-clean and chemically-etched Cu single crystal surfaces

MPS-Authors
/persons/resource/persons227612

Scholten,  Fabian
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons261323

Nguyen,  Khanh-Ly Claudia
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons244746

Bruce,  Jared P.
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons21628

Heyde,  Markus
Interface Science, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons22020

Roldan Cuenya,  Beatriz
Interface Science, Fritz Haber Institute, Max Planck Society;

External Resource
No external resources are shared
Fulltext (public)

ange.202103102.pdf
(Publisher version), 2MB

Supplementary Material (public)
There is no public supplementary material available
Citation

Scholten, F., Nguyen, K.-L.-C., Bruce, J. P., Heyde, M., & Roldan Cuenya, B. (2021). Identifying structure-selectivity correlations in the electrochemical reduction of CO2: a comparison of well-ordered atomically-clean and chemically-etched Cu single crystal surfaces. Angewandte Chemie, 133(35), 19318-19324. doi:10.1002/ange.202103102.


Cite as: http://hdl.handle.net/21.11116/0000-0008-9D0B-C
Abstract
Despite significant theoretical efforts, the identification of the active sites for the electrochemical reduction of CO2 (CO2RR) to specific chemical products has remained elusive. This is partially due to insufficient experimental data gathered on clean and atomically well-ordered electrode surfaces. Here, ultrahigh vacuum based preparation methods and surface science characterization techniques are used together with gas chromatography to demonstrate that subtle changes in the preparation of well-oriented Cu(100) and Cu(111) single crystal surfaces drastically affect their CO2RR selectivity. Copper single crystals with clean, flat, and atomically ordered surfaces are theoretically predicted to yield hydrocarbons. However, these were found experimentally to favour the production of H2. Only when roughness and defects are introduced, for example through an electrochemical etchingor a plasmatreatment, significant amounts of hydrocarbons are generated. These results clearly indicate that structural and morphological effects are the key factors determining the catalytic selectivity of CO2RR.