Bibliographic Details
| Title: |
Robust Fe-N4-C6O2 single atom sites for efficient PMS activation and enhanced FeIV = O reactivity |
| Authors: |
Tiantian Chen, Ganbing Zhang, Hongwei Sun, Yetong Hua, Shu Yang, Dandan Zhou, Haoxin Di, Yiling Xiong, Shenghuai Hou, Hui Xu, Lizhi Zhang |
| Source: |
Nature Communications, Vol 16, Iss 1, Pp 1-12 (2025) |
| Publisher Information: |
Nature Portfolio, 2025. |
| Publication Year: |
2025 |
| Collection: |
LCC:Science |
| Subject Terms: |
Science |
| More Details: |
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. |
| Document Type: |
article |
| File Description: |
electronic resource |
| Language: |
English |
| ISSN: |
2041-1723 |
| Relation: |
https://doaj.org/toc/2041-1723 |
| DOI: |
10.1038/s41467-025-57643-7 |
| Access URL: |
https://doaj.org/article/a0626c3fcb6e442aadfa665b5f03bd20 |
| Accession Number: |
edsdoj.0626c3fcb6e442aadfa665b5f03bd20 |
| Database: |
Directory of Open Access Journals |
