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Restructuring and Activation of Cu(111) under Electrocatalytic Reduction Conditions
Dongfang Cheng1, Ziyang Wei2, Zisheng Zhang2
1Department of Chemical and Biomolecular Engineering, University of California, Los Angeles, CA 90095, USA.
Angewandte Chemie (International Ed. in English)
|March 16, 2023
Summary
Copper surfaces dynamically restructure under electroreduction, forming highly active adatom sites. This restructuring, driven by hydrogen adsorption and electrode potential, is crucial for enhancing the hydrogen evolution reaction.
Area of Science:
- Surface science
- Electrocatalysis
- Computational chemistry
Background:
- Understanding dynamic surface restructuring of copper (Cu) under electroreduction is vital for advancing electrocatalysis.
- The Cu(111) electrode's behavior under reductive conditions is of fundamental scientific interest.
Purpose of the Study:
- To elucidate the structural dynamics of a Cu(111) electrode during electroreduction.
- To investigate the influence of electrode potential and pH on Cu(111) restructuring in acidic media.
Main Methods:
- Joint application of first-principles calculations and operando electrochemical scanning tunneling microscopy (ECSTM).
- Utilized global optimization and grand canonical density functional theory (DFT) for detailed analysis.
Main Results:
- Identified potential- and pH-dependent restructuring of Cu(111) in acidic electrolyte.
- Observed high density of hydrogen (H) atom adsorption and formation of Cu adatoms in a (4×4) superstructure below a threshold potential.
- Determined that strong H adsorption, induced by electrode potential, drives surface restructuring, creating highly active Cu adatom sites.
Conclusions:
- Electrode potential and H adsorption are key drivers for Cu(111) surface restructuring during electroreduction.
- The restructured surface exhibits significantly lower barriers for hydrogen evolution reaction (HER) steps.
- Electrocatalytic activity is enhanced by the in-situ formation of active Cu adatom sites.
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