The DOI matches its Crossref record; 5 of the 5 references it cites were found in a registry or an index.
Metal–Organic Frameworks Mediate Cu Coordination for Selective CO2 Electroreduction
Abstract
The electrochemical carbon dioxide reduction reaction (CO 2 RR) produces diverse chemical species. Cu clusters with a judiciously controlled surface coordination number (CN) provide active sites that simultaneously optimize selectivity, activity, and efficiency for CO 2 RR. Here we report a strategy involving metal–organic framework (MOF)-regulated Cu cluster formation that shifts CO 2 electroreduction toward multiple-carbon product generation. Specifically, we promoted undercoordinated sites during the formation of Cu clusters by controlling the structure of the Cu dimer, the precursor for Cu clusters. We distorted the symmetric paddle-wheel Cu dimer secondary building block of HKUST-1 to an asymmetric motif by separating adjacent benzene tricarboxylate moieties using thermal treatment. By varying materials processing conditions, we modulated the asymmetric local atomic structure, oxidation state and bonding strain of Cu dimers. Using electron paramagnetic resonance (EPR) and in situ X-ray absorption spectroscopy (XAS) experiments, we observed the formation of Cu clusters with low CN from distorted Cu dimers in HKUST-1 during CO 2 electroreduction. These exhibited 45% C 2 H 4 faradaic efficiency (FE), a record for MOF-derived Cu cluster catalysts. A structure–activity relationship was established wherein the tuning of the Cu–Cu CN in Cu clusters determines the CO 2 RR selectivity.
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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
Self-citationEnhanced electrocatalytic CO2 reduction via field-induced reagent concentration
Liu, M., Pang, Y., Zhang, B., De Luna, P., Voznyy, O., Xu, J., Zheng, X., Dinh, C. T., Fan, F., Cao, C., et al. (2016) · Nature · doi:10.1038/nature19060 · Cited by 2,000
Self-citationHighly 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
De Luna, P., Quintero-Bermudez, R., Dinh, C.-T., Ross, M. B., Bushuyev, O. S., Todorović, P., Regier, T., Kelley, S. O., Yang, P., & Sargent, E. H. (2018) · Nature Catalysis · doi:10.1038/s41929-017-0018-9 · Cited by 1,046
Self-citationEnhanced Electrochemical Methanation of Carbon Dioxide with a Dispersible Nanoscale Copper Catalyst
Manthiram, K., Beberwyck, B. J., & Alivisatos, A. P. (2014) · Journal of the American Chemical Society · doi:10.1021/ja5065284 · Cited by 546
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Electrocatalytic reduction of carbon dioxide: opportunities with heterogeneous molecular catalysts
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Metadata
- Authors
- Nam, D.-H., Bushuyev, O. S., Li, J., De Luna, P., Seifitokaldani, A., Dinh, C.-T., García de Arquer, F. P., Wang, Y., Liang, Z., Proppe, A. H., Tan, C. S., Todorović, P., Shekhah, O., Gabardo, C. M., Jo, J. W., Choi, J., Choi, M.-J., Baek, S.-W., Kim, J., Sinton, D., Kelley, S. O., Eddaoudi, M., & Sargent, E. H.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2018-08-16
- Volume
- 140
- Issue
- 36
- Pages
- 11378-11386
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2887717461
- Cited by
- 505
- References
- 5
- FWCI
- 9.33
- Type
- journal article
- Language
- en
- Open access
- closed
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- Nam, D.-H., Bushuyev, O. S., Li, J., De Luna, P., Seifitokaldani, A., Dinh, C.-T., García de Arquer, F. P., Wang, Y., Liang, Z., Proppe, A. H., Tan, C. S., Todorović, P., Shekhah, O., Gabardo, C. M., Jo, J. W., Choi, J., Choi, M.-J., Baek, S.-W., Kim, J., . . . Sargent, E. H. (2018). Metal–Organic Frameworks Mediate Cu Coordination for Selective CO2 Electroreduction. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.8b06407
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