The DOI matches its Crossref record; 50 of the 50 references it cites were found in a registry or an index.
Revealing the CO Coverage-Driven C–C Coupling Mechanism for Electrochemical CO2 Reduction on Cu2O Nanocubes via Operando Raman Spectroscopy
Open accessAbstract
High Resolution Image Download MS PowerPoint Slide Electrochemical reduction of carbon dioxide (CO 2 RR) is an attractive route to close the carbon cycle and potentially turn CO 2 into valuable chemicals and fuels. However, the highly selective generation of multicarbon products remains a challenge, suffering from poor mechanistic understanding. Herein, we used operando Raman spectroscopy to track the potential-dependent reduction of Cu 2 O nanocubes and the surface coverage of reaction intermediates. In particular, we discovered that the potential-dependent intensity ratio of the Cu–CO stretching band to the CO rotation band follows a volcano trend similar to the CO 2 RR Faradaic efficiency for multicarbon products. By combining operando spectroscopic insights with Density Functional Theory, we proved that this ratio is determined by the CO coverage and that a direct correlation exists between the potential-dependent CO coverage, the preferred C–C coupling configuration, and the selectivity to C 2+ products. Thus, operando Raman spectroscopy can serve as an effective method to quantify the coverage of surface intermediates during an electrocatalytic reaction.
Overview
The claims and statistics of this paper haven’t been checked yet.
Run the check — free, no account needed. It reads the open-access text and checks the sources it cites.
Integrity signals
Registry
Cites
Statistics
Verification
Claims the paper makes
The claims and statistics of this paper haven’t been checked yet.
Run the check — free, no account needed. It reads the open-access text and checks the sources it cites.
Self-check
Percentages, sums and reported differences re-computed from the paper’s own numbers.
The self-check needs the paper’s full text.
Citations
Cites
Progress and perspectives of electrochemical CO2 reduction on copper in aqueous electrolyte
Nitopi, S., Bertheussen, E., Scott, S. B., Liu, X., Engstfeld, A. K., Horch, S., Seger, B., Stephens, I. E. L., Chan, K., Hahn, C., et al. (2019) · Chemical Reviews · doi:10.1021/acs.chemrev.8b00705 · Cited by 5,223
How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuels
Peterson, A. A., Abild-Pedersen, F., Studt, F., Rossmeisl, J., & Nørskov, J. K. (2010) · Energy & Environmental Science · doi:10.1039/c0ee00071j · Cited by 3,784
What would it take for renewably powered electrosynthesis to displace petrochemical processes?
De Luna, P., Hahn, C., Higgins, D., Jaffer, S. A., Jaramillo, T. F., & Sargent, E. H. (2019) · Science · doi:10.1126/science.aav3506 · Cited by 3,052
Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels
Birdja, Y. Y., Pérez-Gallent, E., Figueiredo, M. C., Göttle, A. J., Calle-Vallejo, F., & Koper, M. T. M. (2019) · Nature Energy · doi:10.1038/s41560-019-0450-y · Cited by 2,747
CO 2 electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface
Dinh, C.-T., Burdyny, T., Kibria, M. G., Seifitokaldani, A., Gabardo, C. M., García de Arquer, F. P., Kiani, A., Edwards, J. P., De Luna, P., Bushuyev, O. S., et al. (2018) · Science · doi:10.1126/science.aas9100 · Cited by 2,515
Catalysts and Reaction Pathways for the Electrochemical Reduction of Carbon Dioxide
Kortlever, R., Shen, J., Schouten, K. J. P., Calle-Vallejo, F., & Koper, M. T. M. (2015) · The Journal of Physical Chemistry Letters · doi:10.1021/acs.jpclett.5b01559 · Cited by 2,175
Electroreduction of carbon monoxide to liquid fuel on oxide-derived nanocrystalline copper
Li, C. W., Ciston, J., & Kanan, M. W. (2014) · Nature · doi:10.1038/nature13249 · Cited by 1,728
Hori, Y., Murata, A., & Takahashi, R. (1989) · Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases · doi:10.1039/f19898502309 · Cited by 1,640
Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products
Gao, D., Arán-Ais, R. M., Jeon, H. S., & Roldan Cuenya, B. (2019) · Nature Catalysis · doi:10.1038/s41929-019-0235-5 · Cited by 1,489
Ma, W., Xie, S., Liu, T., Fan, Q., Ye, J., Sun, F., Jiang, Z., Zhang, Q., Cheng, J., & Wang, Y. (2020) · Nature Catalysis · doi:10.1038/s41929-020-0450-0 · Cited by 1,468
Molecular tuning of CO2-to-ethylene conversion
Li, F., Thevenon, A., Rosas-Hernández, A., Wang, Z., Li, Y., Gabardo, C. M., Ozden, A., Dinh, C. T., Li, J., Wang, Y., et al. (2020) · Nature · doi:10.1038/s41586-019-1782-2 · Cited by 1,275
Theoretical Insights into a CO Dimerization Mechanism in CO2 Electroreduction
Montoya, J. H., Shi, C., Chan, K., & Nørskov, J. K. (2015) · The Journal of Physical Chemistry Letters · doi:10.1021/acs.jpclett.5b00722 · Cited by 860
Dong, J.-C., Zhang, X.-G., Briega-Martos, V., Jin, X., Yang, J., Chen, S., Yang, Z.-L., Wu, D.-Y., Feliu, J. M., Williams, C. T., et al. (2018) · Nature Energy · doi:10.1038/s41560-018-0292-z · Cited by 789
Arán-Ais, R. M., Scholten, F., Kunze, S., Rizo, R., & Roldan Cuenya, B. (2020) · Nature Energy · doi:10.1038/s41560-020-0594-9 · Cited by 771
Understanding heterogeneous electrocatalytic carbon dioxide reduction through operando techniques
Handoko, A. D., Wei, F., Jenndy, Yeo, B. S., & Seh, Z. W. (2018) · Nature Catalysis · doi:10.1038/s41929-018-0182-6 · Cited by 728
Ren, D., Ang, B. S.-H., & Yeo, B. S. (2016) · ACS Catalysis · doi:10.1021/acscatal.6b02162 · Cited by 721
Huang, Y., Handoko, A. D., Hirunsit, P., & Yeo, B. S. (2017) · ACS Catalysis · doi:10.1021/acscatal.6b03147 · Cited by 685
Efficient electrically powered CO2-to-ethanol via suppression of deoxygenation
Wang, X., Wang, Z., García de Arquer, F. P., Dinh, C.-T., Ozden, A., Li, Y. C., Nam, D.-H., Li, J., Liu, Y.-S., Wicks, J., et al. (2020) · Nature Energy · doi:10.1038/s41560-020-0607-8 · Cited by 666
Managing the Computational Chemistry Big Data Problem: The ioChem-BD Platform
Álvarez-Moreno, M., de Graaf, C., López, N., Maseras, F., Poblet, J. M., & Bo, C. (2015) · Journal of Chemical Information and Modeling · doi:10.1021/ci500593j · Cited by 646
Self-citationCopper nanoparticle ensembles for selective electroreduction of CO 2 to C 2 –C 3 products
Kim, D., Kley, C. S., Li, Y., & Yang, P. (2017) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.1711493114 · Cited by 645
Liu, Z.-P., & Hu, P. (2003) · Journal of the American Chemical Society · doi:10.1021/ja0207551 · Cited by 620
On the origin of the elusive first intermediate of CO 2 electroreduction
Chernyshova, I. V., Somasundaran, P., & Ponnurangam, S. (2018) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.1802256115 · Cited by 555
Strategies to break linear scaling relationships
Pérez-Ramírez, J., & López, N. (2019) · Nature Catalysis · doi:10.1038/s41929-019-0376-6 · Cited by 528
Self-citationGao, J., Zhang, H., Guo, X., Luo, J., Zakeeruddin, S. M., Ren, D., & Grätzel, M. (2019) · Journal of the American Chemical Society · doi:10.1021/jacs.9b07415 · Cited by 495
Gao, D., Zegkinoglou, I., Divins, N. J., Scholten, F., Sinev, I., Grosse, P., & Roldan Cuenya, B. (2017) · ACS Nano · doi:10.1021/acsnano.7b01257 · Cited by 458
Grosse, P., Gao, D., Scholten, F., Sinev, I., Mistry, H., & Roldan Cuenya, B. (2018) · Angewandte Chemie International Edition · doi:10.1002/anie.201802083 · Cited by 425
Wang, X., de Araújo, J. F., Ju, W., Bagger, A., Schmies, H., Kühl, S., Rossmeisl, J., & Strasser, P. (2019) · Nature Nanotechnology · doi:10.1038/s41565-019-0551-6 · Cited by 424
Self-citationConstraining CO coverage on copper promotes high-efficiency ethylene electroproduction
Li, J., Wang, Z., McCallum, C., Xu, Y., Li, F., Wang, Y., Gabardo, C. M., Dinh, C.-T., Zhuang, T.-T., Wang, L., et al. (2019) · Nature Catalysis · doi:10.1038/s41929-019-0380-x · Cited by 391
Tian, Z.-Q., & Ren, B. (2004) · Annual Review of Physical Chemistry · doi:10.1146/annurev.physchem.54.011002.103833 · Cited by 363
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) · Angewandte Chemie International Edition · doi:10.1002/anie.202104114 · Cited by 353
CO-CO coupling on Cu facets: Coverage, strain and field effects
Sandberg, R. B., Montoya, J. H., Chan, K., & Nørskov, J. K. (2016) · Surface Science · doi:10.1016/j.susc.2016.08.006 · Cited by 344
Gunathunge, C. M., Li, X., Li, J., Hicks, R. P., Ovalle, V. J., & Waegele, M. M. (2017) · The Journal of Physical Chemistry C · doi:10.1021/acs.jpcc.7b03910 · Cited by 343
Existence of an Electrochemically Inert CO Population on Cu Electrodes in Alkaline pH
Gunathunge, C. M., Ovalle, V. J., Li, Y., Janik, M. J., & Waegele, M. M. (2018) · ACS Catalysis · doi:10.1021/acscatal.8b01552 · Cited by 315
Electrochemical CO2 Reduction: Classifying Cu Facets
Bagger, A., Ju, W., Varela, A. S., Strasser, P., & Rossmeisl, J. (2019) · ACS Catalysis · doi:10.1021/acscatal.9b01899 · Cited by 294
Bodappa, N., Su, M., Zhao, Y., Le, J.-B., Yang, W.-M., Radjenovic, P., Dong, J.-C., Cheng, J., Tian, Z.-Q., & Li, J.-F. (2019) · Journal of the American Chemical Society · doi:10.1021/jacs.9b04638 · Cited by 274
New aspects of operando Raman spectroscopy applied to electrochemical CO2 reduction on Cu foams
Jiang, S., Klingan, K., Pasquini, C., & Dau, H. (2019) · The Journal of Chemical Physics · doi:10.1063/1.5054109 · Cited by 253
Speciation of Cu Surfaces During the Electrochemical CO Reduction Reaction
Zhao, Y., Chang, X., Malkani, A. S., Yang, X., Thompson, L., Jiao, F., & Xu, B. (2020) · Journal of the American Chemical Society · doi:10.1021/jacs.0c02354 · Cited by 245
CO2 Reduction on Cu at Low Overpotentials with Surface-Enhanced in Situ Spectroscopy
Heyes, J., Dunwell, M., & Xu, B. (2016) · The Journal of Physical Chemistry C · doi:10.1021/acs.jpcc.6b03065 · Cited by 221
Determination of Site Specific Adsorption Energies of CO on Copper
Vollmer, S., Witte, G., & Wöll, C. (2001) · Catalysis Letters · doi:10.1023/a:1012755616064 · Cited by 196
Bond Activation at Monatomic Steps: NO Dissociation at Corrugated Ru(0001)
Hammer, B. (1999) · Physical Review Letters · doi:10.1103/physrevlett.83.3681 · Cited by 189
Oxygen induced promotion of electrochemical reduction of CO2 via co-electrolysis
He, M., Li, C., Zhang, H., Chang, X., Chen, J. G., Goddard, W. A., Cheng, M.-J., Xu, B., & Lu, Q. (2020) · Nature Communications · doi:10.1038/s41467-020-17690-8 · Cited by 183
Moradzaman, M., & Mul, G. (2021) · ChemElectroChem · doi:10.1002/celc.202001598 · Cited by 179
Smith, B. D., Irish, D. E., Kedzierzawski, P., & Augustynski, J. (1997) · Journal of The Electrochemical Society · doi:10.1149/1.1838180 · Cited by 162
Active and Selective Ensembles in Oxide-Derived Copper Catalysts for CO2 Reduction
Dattila, F., García‐Muelas, R., & López, N. (2020) · ACS Energy Letters · doi:10.1021/acsenergylett.0c01777 · Cited by 148
Self-citationCO adsorption on Cu(111) and Cu(001) surfaces: Improving site preference in DFT calculations
Gajdoš, M., & Häfner, J. (2005) · Surface Science · doi:10.1016/j.susc.2005.04.047 · Cited by 140
Revealing the Predominant Surface Facets of Rough Cu Electrodes under Electrochemical Conditions
Gunathunge, C. M., Li, J., Li, X., Hong, J. J., & Waegele, M. M. (2020) · ACS Catalysis · doi:10.1021/acscatal.9b05532 · Cited by 113
Controllable CO adsorption determines ethylene and methane productions from CO2 electroreduction
Bai, H., Cheng, T., Li, S., Zhou, Z., Yang, H., Li, J., Xie, M., Ye, J., Ji, Y., Li, Y., et al. (2020) · 中国科学通报：英文版 · doi:10.1016/j.scib.2020.06.023 · Cited by 104
Velasco‐Vélez, J., Chuang, C., Gao, D., Zhu, Q., Ivanov, D., Jeon, H. S., Arrigo, R., Mom, R. V., Stotz, E., Wu, H., et al. (2020) · ACS Catalysis · doi:10.1021/acscatal.0c03484 · Cited by 84
Self-citationAkemann, W., & Otto, A. (1993) · Surface Science · doi:10.1016/0039-6028(93)90751-5 · Cited by 37
Zhang, P., Cai, J., Chen, Y., Tang, Z., Chen, D., Yang, J., Wu, D., Ren, B. W., & Tian, Z. (2009) · The Journal of Physical Chemistry C · doi:10.1021/jp908478m · Cited by 36
Cited by
Bai, L., Franco, F., Timoshenko, J., Rettenmaier, C., Scholten, F., Jeon, H. S., Yoon, A., Rüscher, M., Herzog, A., Haase, F. T., et al. (2024) · Journal of the American Chemical Society · doi:10.1021/jacs.3c13288 · Cited by 473
Self-citationAtomic-scale surface restructuring of copper electrodes under CO2 electroreduction conditions
Amirbeigiarab, R., Tian, J., Herzog, A., Qiu, C., Bergmann, A., Roldan Cuenya, B., & Magnussen, O. M. (2023) · Nature Catalysis · doi:10.1038/s41929-023-01009-z · Cited by 331
Self-citationYan, T., Chen, X., Kumari, L., Lin, J., Li, M., Fan, Q., Chi, H., Meyer, T. J., Zhang, S., & Ma, X. (2023) · Chemical Reviews · doi:10.1021/acs.chemrev.2c00514 · Cited by 328
Jiang, M., Wang, H., Zhu, M., Luo, X., He, Y., Wang, M., Wu, C., Zhang, L., Li, X., Liao, X., et al. (2024) · Chemical Society Reviews · doi:10.1039/d3cs00857f · Cited by 299
Zhao, Y., Zhang, X.-G., Bodappa, N., Yang, W.-M., Liang, Q., Radjenovica, P. M., Wang, Y.-H., Zhang, Y.-J., Dong, J.-C., Tian, Z.-Q., et al. (2022) · Energy & Environmental Science · doi:10.1039/d2ee01334g · Cited by 293
Metadata
- Authors
- Zhan, C., Dattila, F., Rettenmaier, C., Bergmann, A., Kühl, S., García-Muelas, R., López, N., & Cuenya, B. R.
- Venue
- ACS Catalysis
- Publisher
- American Chemical Society (ACS)
- Published
- 2021-06-11
- Volume
- 11
- Issue
- 13
- Pages
- 7694-7701
- ISSN
- 2155-5435 (ISSN-L)
- OpenAlex
- W3170156421
- Cited by
- 554
- References
- 50
- FWCI
- 12.80
- Type
- journal article
- Language
- en
- Open access
- hybrid
About these checks
Registry, retraction, Cites and statistics results are computed, not judged, with one exception: a printed reference that no index lists is read once by a model before it counts as a citation error. Claims are extracted by a model and kept only when their quote appears verbatim in the text; each cited source is then checked, with a model’s help, for whether it says what the claim relies on. Those verdicts can be wrong — read the claim’s quote and the cited source before relying on one.
Statistics and arithmetic are recomputed, not judged.
Confidence bands are shown only for fields calibrated on our annotated test set. None is calibrated yet, so no band is shown.
What counts as a claim ›How we measure confidence ›How we check this ›
Are you an author, or do you see a problem with this page? Request a review
Data sources
Bibliographic data: Semantic Scholar, OpenAlex, Crossref.
Contains information from the Semantic Scholar Academic Graph Datasets, made available under the ODC Attribution License (ODC-BY 1.0).
Semantic Scholar’s data is described in: Kinney, R., et al. (2023). The Semantic Scholar Open Data Platform. arXiv:2301.10140.
