Long-range interactions driving neighboring Fe–N4 sites in Fenton-like reactions for sustainable water decontamination
Zelin Wu, Zhaokun Xiong, Bingkun Huang, Gang Yao, Sihui Zhan, Bo Lai
Abstract
Actualizing efficient and sustainable environmental catalysis is essential in global water pollution control. The single-atom Fenton-like process, as a promising technique, suffers from reducing potential environmental impacts of single-atom catalysts (SACs) synthesis and modulating functionalized species beyond the first coordination shell. Herein, we devised a high-performance SAC possessing impressive Fenton-like reactivity and extended stability by constructing abundant intrinsic topological defects within carbon planes anchored with Fe−N4 sites. Coupling atomic Fe−N4 moieties and adjacent intrinsic defects provides potent synergistic interaction. Density functional theory calculations reveal that the intrinsic defects optimize the d-band electronic structure of neighboring Fe centers through long-range interactions, consequently boosting the intrinsic activity of Fe−N4 sites. Life cycle assessment and long-term steady operation at the device level indicate promising industrial-scale treatment capability for actual wastewater. This work emphasizes the feasibility of synergistic defect engineering for refining single-atom Fenton-like chemistry and inspires rational materials design toward sustainable environmental remediation. Non-metallic functionalized species in single-atom catalysts potentially contribute to catalytic performance. Herein, the authors report a long range interaction induced by intrinsic carbon defects to enhance the Fenton-like reactivity and stability of adjacent single-atom sites.