Chinese Journal of Catalysis, 2026, 82, 187–200
FeNi nanoparticles cooperate with single-atom sites to drive non-radical fenton-like catalysis: Dominant singlet oxygen and electron transfer pathways for efficient wastewater purification
Heterogeneous Fenton-like systems provide sustainable water-purification solutions; however, improving their catalytic efficiency and recyclability remains challenging. We developed a facile strategy to prepare an FeNi nanoparticle (NPs)-coupled single-atom site catalyst ([FeNi]NPs,SAs-N-C), which exhibits a strong synergy between FeNi NPs and monodisperse Fe/Ni active sites. This catalyst effectively activates peroxomonosulfate (PMS) at low concentrations (0.2 mmol/L), generating abundant reactive oxygen species. Under the condition of continuous flow, the optimized system achieved over 99% sulfamethazine degradation within 3000 min, with a kinetic rate constant (k = 1.5758 min⁻¹) that is 16, 17, and 7 times higher than those of MIL-88B(Fe), MIL-88B(Fe,Ni) and FeNPs,SAs-N-C, respectively. Mechanistic studies showed that PMS activation occurs via a nonradical pathway dominated by singlet oxygen (¹O₂) and direct electron transfer, enhancing the resistance to interference from inorganic anions and natural organic matter. Density functional theory calculations showed that FeNi NPs donated electrons to affect the d orbitals in Fe single-atom sites, enhancing their interaction with PMS to produce ¹O₂ and enable electron transfer. This study presents a viable method for creating efficient NPs coupled with single-atom site catalysts for environmental clean-up.
EClassical 3200 HPLC system equipped with a quaternary pump, online degasser, UV detector, and thermostatically controlled column compartment.
The EClassical 3200 HPLC system was used to quantify the residual concentration of sulfamethazine (SMZ) during the catalytic degradation experiments. It enabled precise monitoring of the degradation kinetics, allowing the determination of conversion rates and kinetic constants to evaluate the catalytic performance of the (FeNi)NPs,SAs-N-C catalyst in the Fenton-like reaction.
