Structure Sensitivity and Catalyst Restructuring for CO2 Electro-reduction on Copper

Dongfang Cheng, Khanh-Ly C. Nguyen, Vaidish Sumaria, Ziyang Wei, Zisheng Zhang, Winston Gee, Yichen Li, Carlos G. Morales-Guio, Markus Heyde, Beatriz Roldan Cuenya, Anastassia N. Alexandrova () and Philippe Sautet ()
Additional contact information
Dongfang Cheng: University of California
Khanh-Ly C. Nguyen: Faradayweg 4-6
Vaidish Sumaria: University of California
Ziyang Wei: University of California
Zisheng Zhang: University of California
Winston Gee: University of California
Yichen Li: University of California
Carlos G. Morales-Guio: University of California
Markus Heyde: Faradayweg 4-6
Beatriz Roldan Cuenya: Faradayweg 4-6
Anastassia N. Alexandrova: University of California
Philippe Sautet: University of California

Nature Communications, 2025, vol. 16, issue 1, 1-14

Abstract: Abstract Cu is the most promising metal catalyst for CO2 electroreduction (CO2RR) to multi-carbon products, yet the structure sensitivity of the reaction and the stability versus restructuring of the catalyst surface under reaction conditions remain controversial. Here, atomic scale simulations of surface energies and reaction pathway kinetics supported by experimental evidence unveil that CO2RR does not take place on perfect planar Cu(111) and Cu(100) surfaces but rather on steps or kinks. These planar surfaces tend to restructure in reaction conditions to the active stepped surfaces, with the strong binding of CO on defective sites acting as a thermodynamic driving force. Notably, we identify that the square motifs adjacent to defects, not the defects themselves, as the active sites for CO2RR via synergistic effect. We evaluate these mechanisms against experiments of CO2RR on ultra-high vacuum-prepared ultraclean Cu surfaces, uncovering the crucial role of step-edge orientation in steering selectivity. Overall, our study refines the structural sensitivity of CO2RR on Cu at the atomic level, highlights the self-activation mechanism and elucidates the origin of in situ restructuring of Cu surfaces during the reaction.

Date: 2025
References: Add references at CitEc
Citations:

Downloads: (external link)
https://www.nature.com/articles/s41467-025-59267-3 Abstract (text/html)

Related works:
This item may be available elsewhere in EconPapers: Search for items with the same title.

Export reference: BibTeX RIS (EndNote, ProCite, RefMan) HTML/Text

Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-59267-3

Ordering information: This journal article can be ordered from
https://www.nature.com/ncomms/

DOI: 10.1038/s41467-025-59267-3

Access Statistics for this article

Nature Communications is currently edited by Nathalie Le Bot, Enda Bergin and Fiona Gillespie

More articles in Nature Communications from Nature
Bibliographic data for series maintained by Sonal Shukla () and Springer Nature Abstracting and Indexing ().