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Modulating the mechanism of electrocatalytic CO2 reduction by cobalt phthalocyanine through polymer coordination and encapsulation
Open accessAbstract
The selective and efficient electrochemical reduction of CO 2 to single products is crucial for solar fuels development. Encapsulating molecular catalysts such as cobalt phthalocyanine within coordination polymers such as poly-4-vinylpyridine leads to dramatically increased activity and selectivity for CO 2 reduction. In this study, we use a combination of kinetic isotope effect and proton inventory studies to explain the observed increase in activity and selectivity upon polymer encapsulation. We provide evidence that axial-coordination from the pyridyl moieties in poly-4-vinylpyridine to the cobalt phthalocyanine complex changes the rate-determining step in the CO 2 reduction mechanism accounting for the increased activity in the catalyst-polymer composite. Moreover, we show that proton delivery to cobalt centers within the polymer is controlled by a proton relay mechanism that inhibits competitive hydrogen evolution. These mechanistic findings provide design strategies for selective CO 2 reduction electrocatalysts and serve as a model for understanding the catalytic mechanism of related heterogeneous systems.
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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
Frontiers, Opportunities, and Challenges in Biochemical and Chemical Catalysis of CO 2 Fixation
Appel, A. M., Bercaw, J. E., Bocarsly, A. B., Dobbek, H., DuBois, D. L., Dupuis, M., Ferry, J. G., Fujita, E., Hille, R., Kenis, P. J. A., et al. (2013) · Chemical Reviews · doi:10.1021/cr300463y · Cited by 2,193
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Cited by
CO 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
Wagner, A., Sahm, C. D., & Reisner, E. (2020) · Nature Catalysis · doi:10.1038/s41929-020-00512-x · Cited by 731
Fu, H. Q., Zhou, M., Liu, P. F., Liu, P., Yin, H., Sun, K. Z., Yang, H. G., Al-Mamun, M., Hu, P., Wang, H.-F., et al. (2022) · Journal of the American Chemical Society · doi:10.1021/jacs.2c01094 · Cited by 508
A Graphene‐Supported Single‐Atom FeN5 Catalytic Site for Efficient Electrochemical CO2 Reduction
Zhang, H., Li, J., Xi, S., Du, Y., Hai, X., Wang, J., Xu, H., Wu, G., Zhang, J., Lu, J., et al. (2019) · Angewandte Chemie International Edition · doi:10.1002/anie.201906079 · Cited by 490
Electrocatalytic reduction of carbon dioxide: opportunities with heterogeneous molecular catalysts
Sun, L., Reddu, V., Fisher, A. C., & Wang, X. (2020) · Energy & Environmental Science · doi:10.1039/c9ee03660a · Cited by 452
Metadata
- Authors
- Liu, Y., & McCrory, C. C. L.
- Venue
- Nature Communications
- Published
- 2019-04-11
- Volume
- 10
- Issue
- 1
- Pages
- 1683-1683
- ISSN
- 2041-1723 (ISSN-L)
- OpenAlex
- W2940051153
- Cited by
- 288
- References
- 4
- FWCI
- 7.01
- Type
- journal article
- Language
- en
- Open access
- gold
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