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Updated: Jun 8, 2025

Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
Published on: April 10, 2018
p-Block metal atom-induced spin state transition of Fe-N-C catalysts for efficient oxygen reduction
Jiana Chen1, Tingyi Zhou1, Changjie He1
1College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, Guangdong 518060, P.R. China. renxz@szu.edu.cn.
Abstract:
A deep understanding of the role of spin configurations of Fe-N-C catalysts in the adsorption and desorption of oxygen intermediates during ORRs is critical for the development of new catalysts for the ORR. Herein, we successfully implanted p-block metal single sites (SnN4, SbN4) into the Fe-N-C system to vary the spin states of Fe species and investigated the ORR performance of active metal centers with varying effective magnetic moments. Through a combination of zero-field cooling (ZFC) temperature-dependent magnetic susceptibility measurements and DFT calculations, we successfully established correlations between the spin state and ORR activity. Magnetic analysis reveals that the p-block metal catalytic sites can effectively induce a low-to-high (or medium) spin state transition of Fe centers. Consequently, the 3d orbital electrons in Fe,M-N-C catalysts penetrate the antibonding π-orbitals of oxygen more easily, thus optimizing the adsorption/desorption of key oxygen intermediates on Fe-N-C catalysts. As a result, the optimized Fe,M-N-C catalyst exhibits a half-wave potential of 0.97 V in a 0.1 M KOH electrolyte, as well as higher durability than conventional Pt/C catalysts. Moreover, the Fe,M-N-C catalysts show encouraging performance in a rechargeable Zn-air battery with high power density and long-term cyclability, indicating the practical applicability of these Fe,M-N-C catalysts.
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