Abstract
Single atom Fe catalysts coordinated with five N atoms (Fe-N5) have been adopted for excellent CO2-to-CO conversion. However, Fe-N5 catalysts typically face trade-offs among Faradaic efficiency (FE), current density, and stability, posing challenges for further commercialization. Additionally, the role of coordinated N species in their catalytic activities remains unclear. Herein, Fe-N5 catalysts coordinated with a high abundance of pyridinic-N (Fe-N5-pyri) or pyrrolic-N (Fe-N5-pyrro) are synthesized. Both operando experiment results and theoretical calculation manifest that pyrrolic-N increases CO2 adsorption capacity, reduces the reaction free energies required for CO2 activation, and facilitates *CO desorption by weakening the bonding strength with reaction centers. As a result, Fe-N5-pyrro exhibits superior CO2-to-CO conversion performance, achieving a maximum FECO of 96.6% and a partial current density exceeding –130mAcm-2 in 0.5M KHCO3, maintaining stable operation for over 100h. This work highlights the role of nitrogen species in Fe-N5 catalysts and provides a promising strategy for synthesizing robust catalyst for CO2 electrochemical reduction.
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