Self-restoration of reactive centers via contaminant-to-catalyst electron replenishment for sustained Fenton-like activity
Abstract
The challenge of achieving self-driven restoration of catalytic sites without external energy or chemical input is critical, which can extend the service life of the catalyst and efficiently reduce water treatment costs. Herein, we fabricate high-spin Mo²⁺ doped FeS₂ catalysts to realize efficient peroxymonosulfate (PMS) activation and contaminant degradation. Notably, doped high-spin Mo²⁺ can spontaneously enrich contaminants and extract electrons from electron-rich contaminants owing to the active 4 d orbital, which replenishes electrons consumed by high-spin Fe during PMS activation. This "contaminant-to-catalyst" electron replenishment pathway, driven primarily by high-spin Mo²⁺ and synergistically assisted by lattice S, accomplishes the sustainable restoration of reactive centers. Consequently, ~800 mg of 0.39 wt% Mo-FeS₂ maintains high activity for over 15 days in a continuous-flow reactor, which treats 216 L of bisphenol A-containing wastewater, surpassing most of reported Fenton-like systems. Ab initio molecular dynamics simulations reveal the interfacial radical oxidation mediated by proton-coupled electron transfer, reducing the migration of radicals and enhancing the mineralization of contaminants. Furthermore, we establish a scalable synthesis for producing kilogram-scale catalyst, immobilizing onto sponges for realizing the selective elimination of trace emerging contaminants from four types of municipal wastewater. Overall, this work provides a promising strategy for developing durable Fenton-like catalysts.
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BibTeX
@article{li2026selfrestoration,
title = {{Self-restoration of reactive centers via contaminant-to-catalyst electron replenishment for sustained Fenton-like activity}},
author = {Yu-Hang Li and Anjie Chen and Xiaoyi Hu and Mingyi Liu and Nan Xu and Alistair G. L. Borthwick and Haodong Ji},
journal = {Nature Communications},
year = {2026},
month = oct,
doi = {10.1038/s41467-026-78165-w},
url = {https://www.nature.com/articles/s41467-026-78165-w},
note = {CC BY-NC-ND 4.0},
}
RIS
TY - JOUR
TI - Self-restoration of reactive centers via contaminant-to-catalyst electron replenishment for sustained Fenton-like activity
AU - Yu-Hang Li
AU - Anjie Chen
AU - Xiaoyi Hu
AU - Mingyi Liu
AU - Nan Xu
AU - Alistair G. L. Borthwick
AU - Haodong Ji
PY - 2026
DA - 2026/10/03
JO - Nature Communications
DO - 10.1038/s41467-026-78165-w
UR - https://www.nature.com/articles/s41467-026-78165-w
AB - The challenge of achieving self-driven restoration of catalytic sites without external energy or chemical input is critical, which can extend the service life of the catalyst and efficiently reduce water treatment costs. Herein, we fabricate high-spin Mo²⁺ doped FeS₂ catalysts to realize efficient peroxymonosulfate (PMS) activation and contaminant degradation. Notably, doped high-spin Mo²⁺ can spontaneously enrich contaminants and extract electrons from electron-rich contaminants owing to the active 4 d orbital, which replenishes electrons consumed by high-spin Fe during PMS activation. This "contaminant-to-catalyst" electron replenishment pathway, driven primarily by high-spin Mo²⁺ and synergistically assisted by lattice S, accomplishes the sustainable restoration of reactive centers. Consequently, ~800 mg of 0.39 wt% Mo-FeS₂ maintains high activity for over 15 days in a continuous-flow reactor, which treats 216 L of bisphenol A-containing wastewater, surpassing most of reported Fenton-like systems. Ab initio molecular dynamics simulations reveal the interfacial radical oxidation mediated by proton-coupled electron transfer, reducing the migration of radicals and enhancing the mineralization of contaminants. Furthermore, we establish a scalable synthesis for producing kilogram-scale catalyst, immobilizing onto sponges for realizing the selective elimination of trace emerging contaminants from four types of municipal wastewater. Overall, this work provides a promising strategy for developing durable Fenton-like catalysts.
SN - 2041-1723
ER -