The DOI matches its Crossref record; 17 of the 17 references it cites were found in a registry or an index.
Efficient Methane Electrosynthesis Enabled by Tuning Local CO2 Availability
Open accessAbstract
The electroreduction of carbon dioxide (CO 2 RR) to valuable chemicals is a promising avenue for the storage of intermittent renewable electricity. Renewable methane, obtained via CO 2 RR using renewable electricity as energy input, has the potential to serve as a carbon-neutral fuel or chemical feedstock, and it is of particular interest in view of the well-established infrastructure for its storage, distribution, and utilization. However, CO 2 RR to methane still suffers from low selectivity at commercially relevant current densities (>100 mA cm –2 ). Density functional theory calculations herein reveal that lowering *CO 2 coverage on the Cu surface decreases the coverage of the *CO intermediate, and then this favors the protonation of *CO to *CHO, a key intermediate for methane generation, compared to the competing step, C–C coupling. We therefore pursue an experimental strategy wherein we control local CO 2 availability on a Cu catalyst by tuning the concentration of CO 2 in the gas stream and regulate the reaction rate through the current density. We achieve as a result a methane Faradaic efficiency (FE) of (48 ± 2)% with a partial current density of (108 ± 5) mA cm –2 and a methane cathodic energy efficiency of 20% using a dilute CO 2 gas stream. We report stable methane electrosynthesis for 22 h. These findings offer routes to produce methane with high FE and high conversion rate in CO 2 RR and also make direct use of dilute CO 2 feedstocks.
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Cites
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What would it take for renewably powered electrosynthesis to displace petrochemical processes?
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CO 2 electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface
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Cited by
Jiao, L., Yang, W., Wan, G., Zhang, R., Zheng, X., Zhou, H., Yu, S., & Jiang, H. (2020) · Angewandte Chemie International Edition · doi:10.1002/anie.202008787 · Cited by 412
Endrődi, B., Kecsenovity, E., Samu, A., Halmágyi, T., Rojas-Carbonell, S., Wang, L., Yan, Y., & Janáky, C. (2020) · Energy & Environmental Science · doi:10.1039/d0ee02589e · Cited by 303
Advanced manufacturing for electrosynthesis of fuels and chemicals from CO 2
Corral, D., Feaster, J. T., Sobhani, S., DeOtte, J. R., Lee, D. U., Wong, A. A., Hamilton, J., Beck, V. A., Sarkar, A., Hahn, C., et al. (2021) · Energy & Environmental Science · doi:10.1039/d0ee03679j · Cited by 98
Metadata
- Authors
- Wang, X., Xu, A., Li, F., Hung, S.-F., Nam, D.-H., Gabardo, C. M., Wang, Z., Xu, Y., Ozden, A., Rasouli, A. S., Ip, A. H., Sinton, D., & Sargent, E. H.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2020-01-28
- Volume
- 142
- Issue
- 7
- Pages
- 3525-3531
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W3003660813
- Cited by
- 264
- References
- 17
- FWCI
- 7.03
- Type
- journal article
- Language
- en
- Open access
- green
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- Wang, X., Xu, A., Li, F., Hung, S.-F., Nam, D.-H., Gabardo, C. M., Wang, Z., Xu, Y., Ozden, A., Rasouli, A. S., Ip, A. H., Sinton, D., & Sargent, E. H. (2020). Efficient Methane Electrosynthesis Enabled by Tuning Local CO2 Availability. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.9b12445
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