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Second‐Sphere Biomimetic Multipoint Hydrogen‐Bonding Patterns to Boost CO2 Reduction of Iron Porphyrins
Open accessAbstract
Inspired by nature's orchestra of chemical subtleties to activate and reduce CO 2, we have developed a family of iron porphyrin derivatives in to which we have introduced urea groups functioning as multipoint hydrogen‐bonding pillars on the periphery of the porphyrinic ring. This structure closely resembles the hydrogen‐bond stabilization scheme of the carbon dioxide (CO 2) adduct in the carbon monoxide dehydrogenase (CODH). We found that such changes to the second coordination sphere significantly lowered the overpotential for CO 2 reduction in this family of molecular catalysts and importantly increased the CO 2 binding rate while maintaining high turnover frequency (TOF) and selectivity. Entrapped water molecules within the molecular clefts were found to be the source of protons for the CO 2 reduction.
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Citations
Cites
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
Cited by
Yi, J., Xie, R., Xie, Z., Chai, G., Liu, T., Chen, R., Huang, Y., & Cao, R. (2020) · Angewandte Chemie International Edition · doi:10.1002/anie.202010601 · Cited by 566
Selectivity in Electrochemical CO2 Reduction
Saha, P., Amanullah, S., & Dey, A. (2022) · Accounts of Chemical Research · doi:10.1021/acs.accounts.1c00678 · Cited by 528
Porphyrin-based frameworks for oxygen electrocatalysis and catalytic reduction of carbon dioxide
Liang, Z., Wang, H.-Y., Zheng, H., Zhang, W., & Cao, R. (2021) · Chemical Society Reviews · doi:10.1039/d0cs01482f · Cited by 506
Metadata
- Authors
- Gotico, P., Boitrel, B., Guillot, R., Sircoglou, M., Quaranta, A., Halime, Z., Leibl, W., & Aukauloo, A.
- Venue
- Angewandte Chemie International Edition
- Publisher
- Wiley
- Published
- 2019-02-20
- Volume
- 58
- Issue
- 14
- Pages
- 4504-4509
- ISSN
- 1433-7851 (ISSN-L)
- 1521-3773
- OpenAlex
- W2916737079
- Cited by
- 188
- References
- 1
- FWCI
- 4.95
- Type
- journal article
- Language
- en
- Open access
- green
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- The paper
- Gotico, P., Boitrel, B., Guillot, R., Sircoglou, M., Quaranta, A., Halime, Z., Leibl, W., & Aukauloo, A. (2019). Second‐Sphere Biomimetic Multipoint Hydrogen‐Bonding Patterns to Boost CO2 Reduction of Iron Porphyrins. Angewandte Chemie International Edition. https://doi.org/10.1002/anie.201814339
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