The DOI matches its Crossref record; 38 of the 38 references it cites were found in a registry or an index.
Strong Hydrogen-Bonded Interfacial Water Inhibiting Hydrogen Evolution Kinetics to Promote Electrochemical CO2 Reduction to C2+
Abstract
Interfacial water is an important participant in electrochemical CO 2 reduction (CO 2 RR), directly affecting the kinetics of hydrogenation steps occurring in the CO 2 RR and competitive hydrogen evolution reaction (HER). However, its structural composition and dynamic evolution are difficult to investigate due to bulk water interference and the bias dependence. Herein, we adopt electrochemical in situ vibration spectroscopy combined with molecular dynamics simulations to probe the dynamic change of interfacial water structure on an electrified hydrophobic electrode surface and further explore the mechanism origin of suppressed HER activity and enhanced multicarbon products’ selectivity. We reveal that interfacial water near the hydrophobic electrode surface exhibits rigid intermolecular hydrogen bonding interaction, and the degree of which increases with a bias potential. The strong intermolecular hydrogen bond makes it hard for water reorientation leading to a longer metal–H distance, which inhibits water dissociation and decreases *H coverage. Moderate *H coverage not only inhibits hydrogen evolution but also ensures hydrogenation of intermediates realizing promoted C–C dimerization. A faradaic efficiency of 75.2% for CO 2 reduction to multicarbon products was ultimately achieved. Our results provide insights into understanding the role of interfacial water structure in controlling reaction selectivity in CO 2 RR.
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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
In situ Raman spectroscopy reveals the structure and dissociation of interfacial water
Wang, Y.-H., Zheng, S., Yang, W.-M., Zhou, R.-Y., He, Q.-F., Radjenovic, P., Dong, J.-C., Li, S., Zheng, J., Yang, Z.-L., et al. (2021) · Nature · doi:10.1038/s41586-021-04068-z · Cited by 1,703
Self-citationStillinger, F. H. (1980) · Science · doi:10.1126/science.209.4455.451 · Cited by 1,128
Zheng, Y., Vasileff, A., Zhou, X., Jiao, Y., Jaroniec, M., & Qiao, S.-Z. (2019) · Journal of the American Chemical Society · doi:10.1021/jacs.9b02124 · Cited by 1,075
Theoretical Considerations on the Electroreduction of CO to C 2 Species on Cu(100) Electrodes
Calle‐Vallejo, F., & Koper, M. T. M. (2013) · Angewandte Chemie International Edition · doi:10.1002/anie.201301470 · Cited by 941
Bio-inspired hydrophobicity promotes CO2 reduction on a Cu surface
Wakerley, D., Lamaison, S., Ozanam, F., Menguy, N., Mercier, D., Marcus, P., Fontecave, M., & Mougel, V. (2019) · Nature Materials · doi:10.1038/s41563-019-0445-x · Cited by 847
In situ probing electrified interfacial water structures at atomically flat surfaces
Li, C.-Y., Le, J.-B., Wang, Y.-H., Chen, S., Yang, Z.-L., Li, J.-F., Cheng, J., & Tian, Z.-Q. (2019) · Nature Materials · doi:10.1038/s41563-019-0356-x · Cited by 789
Self-citationElectrocatalytic reduction of CO2 and CO to multi-carbon compounds over Cu-based catalysts
Ma, W., He, X., Wang, W., Xie, S., Zhang, Q., & Wang, Y. (2021) · Chemical Society Reviews · doi:10.1039/d1cs00535a · Cited by 721
Self-citationXing, Z., Hu, L., Ripatti, D. S., Hu, X., & Feng, X. (2021) · Nature Communications · doi:10.1038/s41467-020-20397-5 · Cited by 664
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Cited by
Zhao, P., Zhang, Y., Chen, B., Zhao, W., Chen, Z., Guan, L., Sun, S., Zhang, S., Li, Y., Peng, W., et al. (2026) · ACS Nano · doi:10.1021/acsnano.6c00124 · Cited by 2
Metadata
- Authors
- Wang, Y., Zhang, J., Zhao, J., Wei, Y., Chen, S., Zhao, H., Su, Y., Ding, S., & Xiao, C.
- Venue
- ACS Catalysis
- Publisher
- American Chemical Society (ACS)
- Published
- 2024-02-19
- Volume
- 14
- Issue
- 5
- Pages
- 3457-3465
- ISSN
- 2155-5435 (ISSN-L)
- OpenAlex
- W4391926255
- Cited by
- 269
- References
- 38
- FWCI
- 17.77
- Type
- journal article
- Language
- en
- Open access
- closed
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- Wang, Y., Zhang, J., Zhao, J., Wei, Y., Chen, S., Zhao, H., Su, Y., Ding, S., & Xiao, C. (2024). Strong Hydrogen-Bonded Interfacial Water Inhibiting Hydrogen Evolution Kinetics to Promote Electrochemical CO2 Reduction to C2+. ACS Catalysis. https://doi.org/10.1021/acscatal.3c05880
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