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Updated: Sep 1, 2025
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Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
Published on: April 10, 2018
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Probing the Dynamics of Low-Overpotential CO2-to-CO Activation on Copper Electrodes with Time-Resolved Raman
Jim de Ruiter1, Hongyu An1, Longfei Wu1
1Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands.
Journal of the American Chemical Society
|August 11, 2022
Summary
Time-resolved spectroscopy reveals how oxide-derived copper electrodes restructure during CO2RR. Pulsed electrolysis activates CO2 to CO at low potentials via dynamic surface changes, offering insights into efficient carbon monoxide production.
Area of Science:
- Electrochemistry
- Materials Science
- Surface Chemistry
Background:
- Oxide-derived copper electrodes enhance CO2RR for valuable chemicals.
- Understanding electrode restructuring during CO2RR is crucial but incomplete.
- The interplay between dynamic restructuring and electrode performance needs elucidation.
Purpose of the Study:
- To investigate the dynamic restructuring of copper (oxide) electrodes during CO2RR.
- To study the adsorption of reaction intermediates using time-resolved surface-enhanced Raman spectroscopy (TR-SERS).
- To correlate electrochemical data with spectral features for mechanistic insights.
Main Methods:
- Utilized time-resolved surface-enhanced Raman spectroscopy (TR-SERS).
- Employed cyclic voltammetry (CV) and pulsed electrolysis (PE) for electrochemical control.
- Coupled electrochemical data with TR-SERS spectral analysis.
Main Results:
- CO2 activation to CO observed during PE at low overpotentials (-0.35 V_RHE) with 10% Faradaic efficiency.
- Stochastic CO intermediates dominate immediately after cathodic bias onset in PE.
- Prolonged low overpotentials suppressed CO intermediates; higher bias (-0.55 V_RHE) formed static CO intermediates.
Conclusions:
- Low-overpotential CO2-to-CO activation is attributed to Cu(111) facet exposure, partially oxidized surfaces, and copper-carbonate-hydroxide intermediates.
- Dynamic restructuring and surface intermediates significantly influence CO2RR activity and selectivity.
- TR-SERS combined with electrochemistry effectively elucidates CO2RR mechanisms.
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