Ren Yi, Li Jun, Liu Chao, Zhang Weiming, Lai Bo
State Key Laboratory of Hydraulics and Mountain River Engineering, Sichuan University, Chengdu, Sichuan 610065, China; College of Water Resource & Hydropower, Sichuan University, Chengdu 610065, China.
State Key Laboratory of Hydraulics and Mountain River Engineering, Sichuan University, Chengdu, Sichuan 610065, China; College of Water Resource & Hydropower, Sichuan University, Chengdu 610065, China.
J Hazard Mater. 2025 Mar 5;485:136799. doi: 10.1016/j.jhazmat.2024.136799. Epub 2024 Dec 14.
Selective oxidation relying on high-valent iron-oxo species (Fe(IV/V)) is a promising way of effective organic decontamination. However, Fe(IV/V) formation and further purposeful reinforcement production are commonly insufficient and unsustainable. Herein, cerium (Ce) modification strategy was adopted for efficient micropollutants removal through boosting Fe(IV/V) generation. Kinetic rate of sulfamethoxazole (SMX) removal through peracetic acid (PAA) activation by FeCe-O-CN is 4.1-fold of that without Ce doping. Ce modification lowered energy barrier of the key reaction pathway (*OH→*O) during Fe(IV/V) formation and accelerated the exposure of the surface Fe site for Fe(IV) production. Steady-state concentration of Fe(IV) and Fe(V) in FeCe-O-CN/PAA process is 2.5 × 10 and 9.7 × 10 M with its corresponding contribution to SMX removal as 64 % and 36 %. Not only intensified SMX removal, Ce modification significantly reduced the toxicity of transformation products. Furthermore, FeCe-O-CN/PAA system satisfies favorable decontaminant in long-term runs, anti-interference, and significantly alleviated bioaccumulation in plants. This study provides a new insight into the association between Ce modification and Fe(IV/V) generation in PAA activation and offered a feasible way for enhanced selective oxidation.
依赖高价铁氧物种（Fe(IV/V)）的选择性氧化是一种很有前景的有效有机净化方法。然而，Fe(IV/V)的形成以及进一步有目的地强化生成通常不足且不可持续。在此，采用铈（Ce）改性策略，通过促进Fe(IV/V)的生成来高效去除微污染物。FeCe-O-CN通过过氧乙酸（PAA）活化去除磺胺甲恶唑（SMX）的动力学速率是未掺杂Ce时的4.1倍。Ce改性降低了Fe(IV/V)形成过程中关键反应途径（*OH→*O）的能垒，并加速了表面铁位点的暴露以生成Fe(IV)。FeCe-O-CN/PAA过程中Fe(IV)和Fe(V)的稳态浓度分别为2.5×10和9.7×10 M，它们对SMX去除的相应贡献分别为64%和36%。Ce改性不仅增强了SMX的去除，还显著降低了转化产物的毒性。此外，FeCe-O-CN/PAA系统在长期运行中具有良好的去污能力、抗干扰能力，并且显著减轻了植物中的生物累积。本研究为Ce改性与PAA活化中Fe(IV/V)生成之间的关联提供了新的见解，并为增强选择性氧化提供了一种可行的方法。
