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, 16631671

DOI: 10.1021/acsenergylett.9b01049


In this work we investigate reaction paths on FeNC 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 FeNx sites convert only CO2CO, 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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