Sulfur Bridge Geometry Boosts Selective Fe<sup>IV</sup>═O Generation for Efficient Fenton‐Like Reactions
High-valent iron-oxo species (Fe<sup>IV</sup>═O) is a fascinating enzymatic agent with excellent anti-interference abilities in various oxidation processes. However, selective and high-yield production of Fe<sup>IV</sup>═O remains challenging. Herein, Fe diatomic pairs are rationally fabricated with an assisted S bridge to tune their neighbor distances and increase their loading to 11.8 wt.%. This geometry regulated the d-band center of Fe atoms, favoring their bonding with the terminal and hydroxyl O sites of peroxymonosulfate (PMS) via heterolytic cleavage of O─O, improving the PMS utilization (70%), and selective generation of Fe<sup>IV</sup>═O (>90%) at a high yield (63% of PMS) offers competitive performance against state-of-the-art catalysts. These continuous reactions in a fabricated device and technol-economic assessment further verified the catalyst with impressive long-term activity and scale-up potential for sustainable water treatment. Altogether, this heteroatom-bridge strategy of diatomic pairs constitutes a promising platform for selective and efficient synthesis of high-valent metal-oxo species.
Authors
- Yi‐Tao Cui (ORCID: https://orcid.org/0000-0001-7104-0059)
- Daohui Lin (ORCID: https://orcid.org/0000-0002-9662-7195)
- Graeme Henkelman (ORCID: https://orcid.org/0000-0002-0336-7153)
- Zhongyuan Guo (ORCID: https://orcid.org/0000-0002-5445-1400)
- Hiroshi Oji (ORCID: https://orcid.org/0000-0002-1183-1390)
- Jiang Xu (ORCID: https://orcid.org/0000-0003-0369-4848)
- Zhiyu Pan (ORCID: https://orcid.org/0000-0001-5736-4495)
- Hao Li (ORCID: https://orcid.org/0000-0002-7577-1366)
- Miao Chen (ORCID: https://orcid.org/0000-0002-3122-7617)
- Xinhua Xu (ORCID: https://orcid.org/0000-0001-7139-1246)
- Yue Chen (ORCID: https://orcid.org/0009-0003-7127-4973)
- Lizhong Zhu (ORCID: https://orcid.org/0000-0001-5044-277X)
- Xunheng Jiang (ORCID: https://orcid.org/0009-0001-5553-1648)
Institutions
- Tohoku University (JP)
- Advanced Institute of Materials Science (JP)
- Shenzhen Institutes of Advanced Technology (CN)
- Nagoya University (JP)
- Zhejiang University (CN)
- The University of Texas at Austin (US)
Publication Details
- Journal
- Advanced Science
- Published
- 2025-03-05
- DOI
- https://doi.org/10.1002/advs.202500313
- Citations
- 18
- Primary Topic
- Advanced oxidation water treatment
- Type
- article
- Field-Weighted Citation Impact
- 14.71
Funders
- National Natural Science Foundation of China
- China Postdoctoral Science Foundation
- National Key Research and Development Program of China