The DOI matches its Crossref record; 8 of the 8 references it cites were found in a registry or an index.
Selectivity Control of Cu Nanocrystals in a Gas-Fed Flow Cell through CO2 Pulsed Electroreduction
Open accessAbstract
In this study, we have taken advantage of a pulsed CO2 electroreduction reaction (CO2RR) approach to tune the product distribution at industrially-relevant current densities in a gas-fed flow cell.We compared the CO2RR selectivity of Cu catalysts subjected to either potentiostatic conditions (fixed applied potential of -0.7 VRHE) or pulsed electrolysis conditions (1 s pulses at oxidative potentials ranging from Ean = 0.6 VRHE to 1.5 VRHE, followed by 1 s pulses at -0.7 VRHE), and identified the main parameters responsible for the enhanced product selectivity observed in the latter case.Herein, two distinct regimes were observed: (i) for Ean = 0.9 VRHE we obtained 10 % enhanced C2 product selectivity (F.E.C2H4 = 43.6% and F.E.C2H5OH = 19.8%)as compared to potentiostatic CO2RR at -0.7 VRHE (F.E.C2H4 = 40.9%and F.E.C2H5OH = 11%), while (ii) for Ean =1.2 VRHE, high CH4 selectivity (F.E.CH4 = 48.3% vs. 0.1% at constant -0.7 VRHE) was observed.Operando spectroscopy (XAS, SERS) and ex-situ microscopy (SEM and TEM) measurements revealed that these differences in catalyst selectivity can be assigned to structural modifications and local pH effects.The morphological reconstruction of the catalyst observed after pulsed electrolysis with Ean = 0.9 VRHE, including the presence of highly defective interfaces and grain boundaries was found to play a key role in the enhancement of the C2 product formation.In turn, pulsed electrolysis with Ean = 1.2 VRHE caused the consumption of OH -species near the catalysts surface, leading to an OH-poor environment favorable for CH4 production.
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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
New insights into the electrochemical reduction of carbon dioxide on metallic copper surfaces
Kuhl, K. P., Cave, E. R., Abram, D. N., & Jaramillo, T. F. (2012) · Energy & Environmental Science · doi:10.1039/c2ee21234j · Cited by 3,160
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
Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene
Mistry, H., Varela, A. S., Bonifacio, C. S., Zegkinoglou, I., Sinev, I., Choi, Y.-W., Kisslinger, K., Stach, E. A., Yang, J. C., Strasser, P., et al. (2016) · Nature Communications · doi:10.1038/ncomms12123 · Cited by 1,214
Self-citationHoang, 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
Self-citationProbing the Active Surface Sites for CO Reduction on Oxide-Derived Copper Electrocatalysts
Verdaguer-Casadevall, A., Li, C. W., Johansson, T. P., Scott, S. B., McKeown, J. T., Kumar, M., Stephens, I. E. L., Kanan, M. W., & Chorkendorff, I. (2015) · Journal of the American Chemical Society · doi:10.1021/jacs.5b06227 · Cited by 645
Investigating the Role of Copper Oxide in Electrochemical CO 2 Reduction in Real Time
Mandal, L., Yang, K. R., Motapothula, M. R., Ren, D., Lobaccaro, P., Patra, A., Sherburne, M., Batista, V. S., Yeo, B. S., Ager, J. W., et al. (2018) · ACS Applied Materials & Interfaces · doi:10.1021/acsami.7b15418 · Cited by 269
Laser-Prepared CuZn Alloy Catalyst for Selective Electrochemical Reduction of CO2 to Ethylene
Feng, Y., Li, Z., Liu, H., Dong, C., Wang, J., Kulinich, S. A., & Du, X. (2018) · Langmuir · doi:10.1021/acs.langmuir.8b02837 · Cited by 164
Cited by
Stabilizing Cu2+ Ions by Solid Solutions to Promote CO2 Electroreduction to Methane
Zhou, X., Shan, J., Chen, L., Xia, B. Y., Ling, T., Duan, J., Jiao, Y., Zheng, Y., & Qiao, S.-Z. (2022) · Journal of the American Chemical Society · doi:10.1021/jacs.1c12212 · Cited by 518
Pulsed Nitrate-to-Ammonia Electroreduction Facilitated by Tandem Catalysis of Nitrite Intermediates
Li, P., Li, R., Liu, Y., Xie, M., Jin, Z., & Yu, G. (2023) · Journal of the American Chemical Society · doi:10.1021/jacs.3c00334 · Cited by 466
Steering the structure and selectivity of CO2 electroreduction catalysts by potential pulses
Timoshenko, J., Bergmann, A., Rettenmaier, C., Herzog, A., Arán-Ais, R. M., Jeon, H. S., Haase, F. T., Hejral, U., Grosse, P., Kühl, S., et al. (2022) · Nature Catalysis · doi:10.1038/s41929-022-00760-z · Cited by 435
Self-citationLai, W., Qiao, Y., Zhang, J., Lin, Z., & Huang, H. (2022) · Energy & Environmental Science · doi:10.1039/d2ee00472k · Cited by 373
Atomic-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
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Metadata
- Authors
- Jeon, H. S., Timoshenko, J., Rettenmaier, C., Herzog, A., Yoon, A., Chee, S. W., Oener, S., Hejral, U., Haase, F. T., & Roldan Cuenya, B.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2021-05-06
- Volume
- 143
- Issue
- 19
- Pages
- 7578-7587
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W3157116955
- Cited by
- 247
- References
- 8
- FWCI
- 6.76
- Type
- journal article
- Language
- en
- Open access
- hybrid
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- Jeon, H. S., Timoshenko, J., Rettenmaier, C., Herzog, A., Yoon, A., Chee, S. W., Oener, S., Hejral, U., Haase, F. T., & Roldan Cuenya, B. (2021). Selectivity Control of Cu Nanocrystals in a Gas-Fed Flow Cell through CO2 Pulsed Electroreduction. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.1c03443
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