The DOI matches its Crossref record; 79 of the 79 references it cites were found in a registry or an index.
Sub‐Second Time‐Resolved Surface‐Enhanced Raman Spectroscopy Reveals Dynamic CO Intermediates during Electrochemical CO2 Reduction on Copper
Open accessAbstract
The electrocatalytic carbon dioxide (CO 2) reduction reaction (CO 2 RR) into hydrocarbons is a promising approach for greenhouse gas mitigation, but many details of this dynamic reaction remain elusive. Here, time‐resolved surface‐enhanced Raman spectroscopy (TR‐SERS) is employed to successfully monitor the dynamics of CO 2 RR intermediates and Cu surfaces with sub‐second time resolution. Anodic treatment at 1.55 V vs. RHE and subsequent surface oxide reduction (below −0.4 V vs. RHE) induced roughening of the Cu electrode surface, which resulted in hotspots for TR‐SERS, enhanced time resolution (down to ≈0.7 s) and fourfold improved CO 2 RR efficiency toward ethylene. With TR‐SERS, the initial restructuring of the Cu surface was followed (<7 s), after which a stable surface surrounded by increased local alkalinity was formed. Our measurements revealed that a highly dynamic CO intermediate, with a characteristic vibration below 2060 cm−1, is related to C−C coupling and ethylene production (−0.9 V vs. RHE), whereas lower cathodic bias (−0.7 V vs. RHE) resulted in gaseous CO production from isolated and static CO surface species with a distinct vibration at 2092 cm−1.
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Cites
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Cited by
The concept of active site in heterogeneous catalysis
Vogt, C., & Weckhuysen, B. M. (2022) · Nature Reviews Chemistry · doi:10.1038/s41570-021-00340-y · Cited by 851
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Metadata
- Authors
- An, H., Wu, L., Mandemaker, L. D. B., Yang, S., de Ruiter, J., Wijten, J. H. J., Janssens, J. C. L., Hartman, T., van der Stam, W., & Weckhuysen, B. M.
- Venue
- Angewandte Chemie International Edition
- Publisher
- Wiley
- Published
- 2021-06-15
- Volume
- 60
- Issue
- 30
- Pages
- 16576-16584
- ISSN
- 1433-7851 (ISSN-L)
- 1521-3773
- OpenAlex
- W3155954709
- Cited by
- 353
- References
- 79
- FWCI
- 9.19
- Type
- journal article
- Language
- en
- Open access
- hybrid
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- An, H., Wu, L., Mandemaker, L. D. B., Yang, S., de Ruiter, J., Wijten, J. H. J., Janssens, J. C. L., Hartman, T., van der Stam, W., & Weckhuysen, B. M. (2021). Sub‐Second Time‐Resolved Surface‐Enhanced Raman Spectroscopy Reveals Dynamic CO Intermediates during Electrochemical CO2 Reduction on Copper. Angewandte Chemie International Edition. https://doi.org/10.1002/anie.202104114
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