Active Sites on Heterogeneous Single-Iron-Atom Electrocatalysts in CO2 Reduction Reaction

By X. Qin, Shangqian Zhu, Fei Xiao, Lulu Zhang, M. Shao. ACS Energy Letters, 2019

156 citations recorded by the source corpus.

Nitrogen-coordinated single-metal-atom catalysts (Me–N–C) are promising candidates for CO2-to-CO electrocatalytic conversion. The nature of real active sites in this type of electrocatalyst, however, is not clear. In this Letter, we study the specific interactions between the reaction intermediates and a model single-iron-atom catalyst (Fe–N–C) by combining in situ infrared absorption spectroscopy and density functional theory (DFT) calculations. For the first time, we confirm that the Fe centers in Fe–N4 moieties hosted by the complete graphitic layer are poisoned by strongly adsorbed CO and should not be the real active sites for gaseous CO production. Further DFT calculation results suggest that the high CO selectivity and reaction rate may originate from Fe–N4 moieties embedded in a defective graphitic layer that have balanced binding energies of adsorbed COOH and CO species. These findings add significant new insights into the mechanisms of CO2 reduction on carbon-based single-atom electrocatalysts.

Subfields: Catalysis, Renewable Energy, Sustainability and the Environment

View Paper: https://www.semanticscholar.org/paper/68be586b9ae688791ca3f04de793d18f5de538ad

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In Catalysis

1. P. Strasser
2. A. Varela
3. Karen Chan
4. J. Rossmeisl
5. A. Bagger
6. B. Roldán Cuenya
7. Jens K. Nørskov

In Renewable Energy, Sustainability and the Environment

1. P. Strasser
2. Karen Chan
3. A. Varela
4. B. Roldán Cuenya
5. I. Stephens
6. J. Rossmeisl
7. M. Koper
8. A. Bagger

Citations in the corpus

• 2022 roadmap on low temperature electrochemical CO2 reduction (2022, methodology): “In-situ IR study combined with DFT simulation proposed the Fe−N4 moiety with the defective graphitic layer as the active site of a Fe–N–C catalyst instead of the Fe center in the complete graphite due to their balanced ∗COOH and ∗CO binding strength [100].”