The DOI matches its Crossref record; 10 of the 10 references it cites were found in a registry or an index.
Unraveling Mechanistic Reaction Pathways of the Electrochemical CO2 Reduction on Fe–N–C Single-Site Catalysts
Abstract
We report a joint experimental–computational mechanistic study of electrochemical reduction of CO 2 to CH 4, catalyzed by solid-state Fe–N–C catalysts, which feature atomically dispersed, catalytically active Fe–N x sites and represent one of the very rare examples of solid, non-Cu-based electrocatalysts that yield hydrocarbon products. Work reported here focuses on the identification of plausible mechanistic pathways from CO 2 to various C 1 products including methane. It is found that Fe–N x sites convert only CO 2, CO, and CH 2 O into methane, whereas CH 3 OH appears to be an end product. Distinctly different pH dependence of the catalytic CH 4 evolution from CH 2 O in comparison with that of CO 2 and CO reduction indicates differences in the proton participation of rate-determining steps. By comparing the experimental observations with density functional theory derived free energy diagrams of reactive intermediates along the CO 2 reduction reaction coordinates, we unravel the dominant mechanistic pathways and roles of CO and CH 2 O during the catalytic CO 2 -to-CH 4 cascades and their rate-determining steps. We close with a comprehensive reaction network of CO 2 RR on single-site Fe–N–C catalysts, which may prove useful in developing efficient, non-Cu-based catalysts for hydrocarbon production.
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Cites
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Self-citationActive and Selective Conversion of CO 2 to CO on Ultrathin Au Nanowires
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Cited by
Metal‐Nitrogen‐Doped Carbon Materials as Highly Efficient Catalysts: Progress and Rational Design
Shi, Z., Yang, W., Gu, Y., Liao, T., & Sun, Z. (2020) · Advanced Science · doi:10.1002/advs.202001069 · Cited by 470
Metadata
- Authors
- Ju, W., Bagger, A., Wang, X., Tsai, Y., Luo, F., Möller, T., Wang, H., Rossmeisl, J., Varela, A. S., & Strasser, P.
- Venue
- ACS Energy Letters
- Publisher
- American Chemical Society (ACS)
- Published
- 2019-06-17
- Volume
- 4
- Issue
- 7
- Pages
- 1663-1671
- ISSN
- 2380-8195 (ISSN-L)
- OpenAlex
- W2953316844
- Cited by
- 188
- References
- 10
- FWCI
- 5.72
- Type
- journal article
- Language
- en
- Open access
- closed
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- Ju, W., Bagger, A., Wang, X., Tsai, Y., Luo, F., Möller, T., Wang, H., Rossmeisl, J., Varela, A. S., & Strasser, P. (2019). Unraveling Mechanistic Reaction Pathways of the Electrochemical CO2 Reduction on Fe–N–C Single-Site Catalysts. ACS Energy Letters. https://doi.org/10.1021/acsenergylett.9b01049
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