Robust Fe-N4-C6O2 single atom sites for efficient PMS activation and enhanced FeIV = O reactivity

Tiantian Chen, Ganbing Zhang (), Hongwei Sun, Yetong Hua, Shu Yang, Dandan Zhou, Haoxin Di, Yiling Xiong, Shenghuai Hou, Hui Xu () and Lizhi Zhang ()
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Tiantian Chen: Central China Normal University
Ganbing Zhang: Hubei University
Hongwei Sun: Central China Normal University
Yetong Hua: Central China Normal University
Shu Yang: Central China Normal University
Dandan Zhou: Central China Normal University
Haoxin Di: Central China Normal University
Yiling Xiong: Central China Normal University
Shenghuai Hou: Central China Normal University
Hui Xu: Central China Normal University
Lizhi Zhang: Shanghai Jiao Tong University

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract The microenvironment regulation of Fe-N4 single atom catalysts (SACs) critically governs peroxymonosulfate (PMS) activation. Although conventional heteroatom substitution in primary coordination enhances activity, it disrupts Fe-N4 symmetry and compromises stability. Herein, we propose oxygen doping in the secondary coordination shell to construct Fe-N4-C6O2 SAC, which amplifies the localized electric field while preserving the pristine coordination symmetry, thus trading off its activity and stability. This approach suppresses Fe-N bond structural deformation (bond amplitude reduced from 0.875–3.175 Å to 0.925–2.975 Å) during PMS activation by lowering Fe center electron density to strengthen Fe-N bond, achieving extended catalytic durability (>240 h). Simultaneously, the weakened coordination field lowers the Fe=O σ* orbital energy, promoting electrophilic σ-attack of high-valent iron-oxo towards bisphenol A, and increasing its degradation rate by 41.6-fold. This work demonstrates secondary coordination engineering as a viable strategy to resolve the activity-stability trade-off in SAC design, offering promising perspectives for developing environmental catalysts.

Date: 2025
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DOI: 10.1038/s41467-025-57643-7

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