The DOI matches its Crossref record; 7 of the 7 references it cites were found in a registry or an index.
Selective CO2 Reduction to CO in Water using Earth-Abundant Metal and Nitrogen-Doped Carbon Electrocatalysts
Abstract
Earth-abundant transition metal (Fe, Co, or Ni) and nitrogen-doped porous carbon electrocatalysts (M-N-C, where M denotes the metal) were synthesized from cheap precursors via silica-templated pyrolysis. The effect of the material composition and structure (i.e., porosity, nitrogen doping, metal identity, and oxygen functionalization) on the activity for the electrochemical CO 2 reduction reaction (CO 2 RR) was investigated. The metal-free N-C exhibits a high selectivity but low activity for CO 2 RR. Incorporation of the Fe and Ni, but not Co, sites in the N-C material is able to significantly enhance the activity. The general selectivity order for CO 2 -to-CO conversion in water is found to be Ni > Fe ≫ Co with respect to the metal in M-N-C, while the activity follows Ni, Fe ≫ Co. Notably, the Ni-doped carbon exhibits a high selectivity with a faradaic efficiency of 93% for CO production. Tafel analysis shows a change of the rate-determining step as the metal overtakes the role of the nitrogen as the most active site. Recording the X-ray photoelectron spectra and extended X-ray absorption fine structure demonstrates that the metals are atomically dispersed in the carbon matrix, most likely coordinated to four nitrogen atoms and with carbon atoms serving as a second coordination shell. Presumably, the carbon atoms in the second coordination shell of the metal sites in M-N-C significantly affect the CO 2 RR activity because the opposite reactivity order is found for carbon supported metal meso-tetraphenylporphyrin complexes. From a better understanding of the relationship between the CO 2 RR activity and the material structure, it becomes possible to rationally design high-performance porous carbon electrocatalysts involving earth-abundant metals for CO 2 valorization.
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Cites
Atomically dispersed Ni(i) as the active site for electrochemical CO2 reduction
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Enhanced electrocatalytic CO2 reduction via field-induced reagent concentration
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Atomic cobalt on nitrogen-doped graphene for hydrogen generation
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Molecular metal–Nx centres in porous carbon for electrocatalytic hydrogen evolution
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Achieving Highly Efficient, Selective, and Stable CO2 Reduction on Nitrogen-Doped Carbon Nanotubes
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Li, X., Yu, J., Jaroniec, M., & Chen, X. (2019) · Chemical Reviews · doi:10.1021/acs.chemrev.8b00400 · Cited by 2,304
Single atom electrocatalysts supported on graphene or graphene-like carbons
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Defect engineering in earth-abundant electrocatalysts for CO2 and N2 reduction
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Stable and Efficient Single-Atom Zn Catalyst for CO2 Reduction to CH4
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Lu, C., Jiang, K., Tranca, D., Wang, N., Zhu, H., Rodríguez-Hernández, F., Chen, Z., Yang, C., Zhang, F., Su, Y., et al. (2021) · Journal of Materials Chemistry A · doi:10.1039/d1ta05990d · Cited by 46
Metadata
- Authors
- Hu, X.-M., Hval, H. H., Bjerglund, E. T., Dalgaard, K. J., Madsen, M. R., Pohl, M.-M., Welter, E., Lamagni, P., Buhl, K. B., Bremholm, M., Beller, M., Pedersen, S. U., Skrydstrup, T., & Daasbjerg, K.
- Venue
- ACS Catalysis
- Publisher
- American Chemical Society (ACS)
- Published
- 2018-06-12
- Volume
- 8
- Issue
- 7
- Pages
- 6255-6264
- ISSN
- 2155-5435 (ISSN-L)
- OpenAlex
- W2807945784
- Cited by
- 344
- References
- 7
- FWCI
- 8.65
- Type
- journal article
- Language
- en
- Open access
- closed
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