The DOI matches its Crossref record; 53 of the 53 references it cites were found in a registry or an index.
Tracking a Common Surface-Bound Intermediate during CO2-to-Fuels Catalysis
Open accessAbstract
Rational design of selective CO2-to-fuels electrocatalysts requires direct knowledge of the electrode surface structure during turnover. Metallic Cu is the most versatile CO2-to-fuels catalyst, capable of generating a wide array of value-added products, including methane, ethylene, and ethanol. All of these products are postulated to form via a common surface-bound CO intermediate. Therefore, the kinetics and thermodynamics of CO adsorption to Cu play a central role in determining fuel-formation selectivity and efficiency, highlighting the need for direct observation of CO surface binding equilibria under catalytic conditions. Here, we synthesize nanostructured Cu films adhered to IR-transparent Si prisms, and we find that these Cu surfaces enhance IR absorption of bound molecules. Using these films as electrodes, we examine Cu-catalyzed CO2 reduction in situ via IR spectroelectrochemistry. We observe that Cu surfaces bind electrogenerated CO, derived from CO2, beginning at -0.60 V vs RHE with increasing surface population at more negative potentials. Adsorbed CO is in dynamic equilibrium with dissolved (13)CO and exchanges rapidly under catalytic conditions. The CO adsorption profiles are pH independent, but adsorbed CO species undergo a reversible transformation on the surface in modestly alkaline electrolytes. These studies establish the potential, concentration, and pH dependencies of the CO surface population on Cu, which serve to maintain a pool of this vital intermediate primed for further reduction to higher order fuel products.
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Cites
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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
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
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The recent development of efficient Earth-abundant transition-metal nanocatalysts
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Metadata
- Authors
- Wuttig, A., Liu, C., Peng, Q., Yaguchi, M., Hendon, C. H., Motobayashi, K., Ye, S., Osawa, M., & Surendranath, Y.
- Venue
- ACS Central Science
- Publisher
- American Chemical Society (ACS)
- Published
- 2016-08-08
- Volume
- 2
- Issue
- 8
- Pages
- 522-528
- ISSN
- 2374-7943 (ISSN-L)
- 2374-7951
- OpenAlex
- W2517552393
- Cited by
- 316
- References
- 53
- FWCI
- 6.79
- Type
- journal article
- Language
- en
- Open access
- diamond
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- Wuttig, A., Liu, C., Peng, Q., Yaguchi, M., Hendon, C. H., Motobayashi, K., Ye, S., Osawa, M., & Surendranath, Y. (2016). Tracking a Common Surface-Bound Intermediate during CO2-to-Fuels Catalysis. ACS Central Science. https://doi.org/10.1021/acscentsci.6b00155
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