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PreprintCC BYChemRxiv

Self-recycling Fenton chemistry through the ordered hydration shells of Fe

  1. 1Research Center of Ministry of Education for Fine Chemicals
  2. 2Shanxi University
  3. 3Key Laboratory of Chemical Biology and Molecular Engineering of Ministry of Education

Abstract

The century-old Fenton reaction has been constrained by the kinetic bottleneck of Fe3+/Fe2+ cycling, which demands excessive iron dosing and generates hazardous sludge. Here we report that Fe3+ ions intrinsically bypass this limitation through a remote through-space ligand effect that induces long-range ordering of water molecules beyond the first coordination shell. This ordered hydration network functions as a visible-to-red-light antenna via a collective water-network-to-metal charge transfer mechanism, continuously generating electrons that reduce Fe3+ to Fe2+ without exogenous photocatalysts or chemical reductants. This self-sustaining cycle achieves approximately 80% TOC removal of phenol in a scaled-up 15 L reactor under natural sunlight and sustains approximately 65% TOC removal over 20 consecutive cycles for real pharmaceutical wastewater, with only 1.2% iron loss per cycle and near-zero sludge generation. This work transforms a canonical kinetic barrier into a self-regenerating catalytic platform, uncovering a hydration-driven photochemical route that offers sustainable, sludge-free, sunlight-driven water purification.

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BibTeX
@misc{zhang2026selfrecycling,
  title = {{Self-recycling Fenton chemistry through the ordered hydration shells of Fe}},
  author = {Qi Zhang and Xuan Guo and Ruihan Wang and Hu Shi and Jie Wang and Jianghong Zhao and Hongxia Zhang and Pengju Yang},
  howpublished = {ChemRxiv},
  year = {2026},
  month = sep,
  doi = {10.26434/chemrxiv.15009323/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009323/v1},
  note = {CC BY},
}
RIS
TY  - UNPB
TI  - Self-recycling Fenton chemistry through the ordered hydration shells of Fe
AU  - Qi Zhang
AU  - Xuan Guo
AU  - Ruihan Wang
AU  - Hu Shi
AU  - Jie Wang
AU  - Jianghong Zhao
AU  - Hongxia Zhang
AU  - Pengju Yang
PY  - 2026
DA  - 2026/09/22
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15009323/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009323/v1
AB  - The century-old Fenton reaction has been constrained by the kinetic bottleneck of Fe3+/Fe2+ cycling, which demands excessive iron dosing and generates hazardous sludge. Here we report that Fe3+ ions intrinsically bypass this limitation through a remote through-space ligand effect that induces long-range ordering of water molecules beyond the first coordination shell. This ordered hydration network functions as a visible-to-red-light antenna via a collective water-network-to-metal charge transfer mechanism, continuously generating electrons that reduce Fe3+ to Fe2+ without exogenous photocatalysts or chemical reductants. This self-sustaining cycle achieves approximately 80% TOC removal of phenol in a scaled-up 15 L reactor under natural sunlight and sustains approximately 65% TOC removal over 20 consecutive cycles for real pharmaceutical wastewater, with only 1.2% iron loss per cycle and near-zero sludge generation. This work transforms a canonical kinetic barrier into a self-regenerating catalytic platform, uncovering a hydration-driven photochemical route that offers sustainable, sludge-free, sunlight-driven water purification.
ER  -