The DOI matches its Crossref record; 9 of the 9 references it cites were found in a registry or an index.
Close to 90% Single-Pass Conversion Efficiency for CO2 Electroreduction in an Acid-Fed Membrane Electrode Assembly
Abstract
The formation of (bi)carbonates is a pressing issue for CO 2 electroreduction in neutral or alkaline solutions. It adversely causes low single-pass conversion efficiency as a result of (bi)carbonate crossover, as well as limited device lifetimes as a result of (bi)carbonate precipitation at the cathode. One emerging solution to circumvent this challenge is conducting the reaction in acids. To this end, we here demonstrate an acid-fed membrane electrode assembly (MEA) for CO 2 electroreduction to CO. A diluted electrolyte with an H + to Cs + ratio of 1:1 and a relatively low current density are optimal conditions to achieve high CO Faradaic efficiencies. A relatively high H + versus Cs + ratio offers high electrocatalytic activities. By systematically evaluating the impact of H + and Cs + concentration on the electrochemical performance, we uncover the essential role of the balance between the rates of (bi)carbonate formation and H + diffusion in determining the selectivity and activity. As a result, we report a CO partial current density of ∼105 mA cm –2 at an ∼4 V cell voltage, a near-doubled activity toward CO compared to a neutral MEA at a similar voltage. Under the optimal conditions for long-term operation, our acid-fed membrane electrode assembly is capable of delivering a CO Faradaic efficiency of ∼80%, an extraordinary single-pass conversion efficiency of ∼90% (about twice that of neutral MEA), and a 50 h long-term stability notably superior to those in previous reports.
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Citations
Cites
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
General Techno-Economic Analysis of CO 2 Electrolysis Systems
Jouny, M., Luc, W., & Jiao, F. (2018) · Industrial & Engineering Chemistry Research · doi:10.1021/acs.iecr.7b03514 · Cited by 1,628
What Should We Make with CO2 and How Can We Make It?
Bushuyev, O. S., De Luna, P., Dinh, C. T., Tao, L., Saur, G., van de Lagemaat, J., Kelley, S. O., & Sargent, E. H. (2018) · Joule · doi:10.1016/j.joule.2017.09.003 · Cited by 1,593
CO 2 electrolysis to multicarbon products at activities greater than 1 A cm −2
García de Arquer, F. P., Dinh, C.-T., Ozden, A., Wicks, J., McCallum, C., Kirmani, A. R., Nam, D.-H., Gabardo, C., Seifitokaldani, A., Wang, X., et al. (2020) · Science · doi:10.1126/science.aay4217 · Cited by 1,517
Self-citationCO 2 electrolysis to multicarbon products in strong acid
Huang, J. E., Li, F., Ozden, A., Sedighian Rasouli, A., García de Arquer, F. P., Liu, S., Zhang, S., Luo, M., Wang, X., Lum, Y., et al. (2021) · Science · doi:10.1126/science.abg6582 · Cited by 1,359
Hoang, T. T. H., Verma, S., Ma, S., Fister, T. T., Timoshenko, J., Frenkel, A. I., Kenis, P. J. A., & Gewirth, A. A. (2018) · Journal of the American Chemical Society · doi:10.1021/jacs.8b01868 · Cited by 852
Technical photosynthesis involving CO2 electrolysis and fermentation
Haas, T., Krause, R., Weber, R., Demler, M., & Schmid, G. (2018) · Nature Catalysis · doi:10.1038/s41929-017-0005-1 · Cited by 649
Verma, S., Hamasaki, Y., Kim, C., Huang, W., Lu, S., Jhong, H.-R. M., Gewirth, A. A., Fujigaya, T., Nakashima, N., & Kenis, P. J. A. (2018) · ACS Energy Letters · doi:10.1021/acsenergylett.7b01096 · Cited by 521
One-step electrosynthesis of ethylene and ethanol from CO2 in an alkaline electrolyzer
Ma, S., Sadakiyo, M., Luo, R., Heima, M., Yamauchi, M., & Kenis, P. J. A. (2016) · Journal of Power Sources · doi:10.1016/j.jpowsour.2015.09.124 · Cited by 488
Cited by
Chang, B., Pang, H., Raziq, F., Wang, S., Huang, K.-W., Ye, J., & Zhang, H. (2023) · Energy & Environmental Science · doi:10.1039/d3ee00964e · Cited by 458
Yan, 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
Metadata
- Authors
- Pan, B., Fan, J., Zhang, J., Luo, Y., Shen, C., Wang, C., Wang, Y., & Li, Y.
- Venue
- ACS Energy Letters
- Publisher
- American Chemical Society (ACS)
- Published
- 2022-10-31
- Volume
- 7
- Issue
- 12
- Pages
- 4224-4231
- ISSN
- 2380-8195 (ISSN-L)
- OpenAlex
- W4307896342
- Cited by
- 236
- References
- 9
- FWCI
- 8.37
- Type
- journal article
- Language
- en
- Open access
- closed
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- Pan, B., Fan, J., Zhang, J., Luo, Y., Shen, C., Wang, C., Wang, Y., & Li, Y. (2022). Close to 90% Single-Pass Conversion Efficiency for CO2 Electroreduction in an Acid-Fed Membrane Electrode Assembly. ACS Energy Letters. https://doi.org/10.1021/acsenergylett.2c02292
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