Unravelling Mechanistic Reaction Pathways of the Electrochemical CO2 Reduction on Fe-N-C Single-Site Catalysts
Wen Ju, Alexander Bagger, Xingli Wang, Yulin Tsai, Fang Luo, Tim Möller, Huan Wang, Jan Rossmeisl, Ana Sofia Varela, and Peter Strasser
ACS Energy Lett. 2019, 4, 1663−1671
DescriptionIn this work we investigate reaction paths on Fe−N−C from CO2 to CH4. The work reported here focuses on the identification of plausible mechanistic pathways from CO2 to various C1 products including methane. It is found that Fe−Nx sites convert only CO2, CO, and CH2O into methane, whereas CH3OH appears to be an end product. By comparing the experimental observations with density functional theory derived free energy diagrams of reactive intermediates along the CO2 reduction reaction coordinates, we unravel the dominant mechanistic pathways and roles of CO and CH2O during the catalytic CO2-to-CH4 cascades and their rate-determining steps.
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