Regulation of coordinated nitrogen species for atomically dispersed Fe-N5 catalyst to boost electrocatalytic CO2-to-CO conversion

Li, Da, Liu, Jiabei, Chen, Xinyi, Feng, Zhiming, Wang, Shaohong, Wang, Yucheng, Lin, Nan, Wu, Jing and Feng, Yujie 2025. Regulation of coordinated nitrogen species for atomically dispersed Fe-N5 catalyst to boost electrocatalytic CO2-to-CO conversion. Applied Catalysis B: Environment and Energy 365 , 124824. 10.1016/j.apcatb.2024.124824 Item availability restricted.

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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 –130 mA cm−2 in 0.5 M KHCO3, maintaining stable operation for over 100 h. 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.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry Cardiff Catalysis Institute (CCI)
Publisher:	Elsevier
ISSN:	0926-3373
Date of First Compliant Deposit:	7 January 2025
Date of Acceptance:	14 November 2024
Last Modified:	08 Jan 2025 12:45
URI:	https://orca.cardiff.ac.uk/id/eprint/175054

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