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Role of Surface Hydroxyls in Atomic-Scale Copper Restructuring during CO Electroreduction.
Jie Wei1,2, Zisheng Zhang3,4, Winston Gee3
1Helmholtz Young Investigator Group Nanoscale Operando CO2 Photo-Electrocatalysis, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, 14109 Berlin, Germany.
Journal of the American Chemical Society
|November 24, 2025
Summary
Surface hydroxyls and CO synergistically restructure copper electrocatalysts during CO2 electroreduction (CO2R). This atomic restructuring generates new active sites, impacting reaction selectivity and kinetics under realistic conditions.
Area of Science:
- Surface science
- Electrocatalysis
- Nanomaterials
Background:
- Electrocatalyst nanoscale structure dictates reaction selectivity and kinetics.
- Evolution of catalyst surfaces under reaction conditions and the role of surface hydroxyls (OHad) are poorly understood.
Purpose of the Study:
- To investigate the dynamic restructuring of copper (Cu) electrocatalysts during CO2 electroreduction (CO2R).
- To elucidate the roles of surface hydroxyls (OHad) and the interfacial microenvironment in Cu surface restructuring.
Main Methods:
- Electrochemical atomic force microscopy (EC-AFM)
- Raman spectroscopy
- Grand canonical modeling
Main Results:
- OHad synergistically interacts with adsorbed CO (COad) to restructure Cu surfaces.
- Restructuring generates Cu adatoms and nanoclusters at mild potentials, which aggregate or dissolve at more negative potentials.
- Surface restructuring leads to low-coordinated Cu sites and disordered interfacial water networks.
Conclusions:
- Surface kinetics and interfacial microenvironments are critical for atomic-scale restructuring of electrocatalysts.
- Findings necessitate a re-evaluation of catalytic surface states under realistic operating conditions.
- Understanding dynamic restructuring is key for designing efficient CO2R electrocatalysts.
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