Inter-site structural heterogeneity induction of single atom Fe catalysts for robust oxygen reduction

Peng Zhang, Hsiao Chien Chen, Houyu Zhu, Kuo Chen, Tuya Li, Yilin Zhao, Jiaye Li, Ruanbo Hu, Siying Huang, Wei Zhu, Yunqi Liu*, Yuan Pan*

*Corresponding author for this work

Research output: Contribution to journalJournal Article peer-review

7 Scopus citations


Metal-nitrogen-carbon catalysts with hierarchically dispersed porosity are deemed as efficient geometry for oxygen reduction reaction (ORR). However, catalytic performance determined by individual and interacting sites originating from structural heterogeneity is particularly elusive and yet remains to be understood. Here, an efficient hierarchically porous Fe single atom catalyst (Fe SAs-HP) is prepared with Fe atoms densely resided at micropores and mesopores. Fe SAs-HP exhibits robust ORR performance with half-wave potential of 0.94 V and turnover frequency of 5.99 e−1s−1site−1 at 0.80 V. Theoretical simulations unravel a structural heterogeneity induced optimization, where mesoporous Fe-N4 acts as real active centers as a result of long-range electron regulation by adjacent microporous sites, facilitating O2 activation and desorption of key intermediate *OH. Multilevel operando characterization results identify active Fe sites undergo a dynamic evolution from basic Fe-N4 to active Fe-N3 under working conditions. Our findings reveal the structural origin of enhanced intrinsic activity for hierarchically porous Fe-N4 sites.

Original languageEnglish
Article number2062
Pages (from-to)2062
JournalNature Communications
Issue number1
StatePublished - 07 03 2024

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© 2024. The Author(s).


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