Advanced Interdisciplinary Institute of Environment and Ecology, Beijing Normal University, Zhu Hai519087, People's Republic of China.
School of Biotechnology and Health Science, Wuyi University, Jiangmen529020, People's Republic of China.
Environ Sci Technol. 2023 Nov 28;57(47):18607-18616. doi: 10.1021/acs.est.2c06414. Epub 2023 Feb 6.
In this study, novel light emitting diode (LED)-activated periodate (PI) advanced oxidation process (AOP) at an irradiation wavelength in the ultraviolet A range (UVA, UVA-LED/PI AOP) was developed and investigated using naproxen (NPX) as a model micropollutant. The UVA-LED/PI AOP remarkably enhanced the degradation of NPX and seven other selected micropollutants with the observed pseudo-first-order rate constants ranging from 0.069 ± 0.001 to 4.50 ± 0.145 min at pH 7.0, demonstrating a broad-spectrum micropollutant degradation ability. Lines of evidence from experimental analysis and kinetic modeling confirmed that hydroxyl radical (OH) and ozone (O) were the dominant species generated in UVA-LED/PI AOP, and they contributed evenly to NPX degradation. Increasing the pH and irradiation wavelength negatively affected NPX degradation, and this could be well explained by the decreased quantum yield (Φ) of PI. The degradation kinetics of NPX by the UVA-LED/PI AOP in the presence of water matrices (i.e., chloride, bicarbonate, and humic acid) and in real waters were examined, and the underlying mechanisms were illustrated. A total of nine transformation products were identified from NPX oxidation by the UVA-LED/PI AOP, mainly via hydroxylation, dealkylation, and oxidation pathways. The UVA-LED/PI AOP proposed might be a promising technology for the treatment of micropollutants in aqueous solutions. The pivotal role of Φ during light photolysis of PI may guide the future design of light-assisted PI AOPs.
在这项研究中,我们开发并研究了一种新型发光二极管(LED)激活过碘酸盐(PI)高级氧化工艺(AOP),其辐照波长在紫外线 A 范围内(UVA,UVA-LED/PI AOP),并以萘普生(NPX)作为模型微量污染物进行研究。UVA-LED/PI AOP 显著增强了 NPX 和其他七种选定的微量污染物的降解,在 pH 值为 7.0 时观察到的拟一级速率常数范围从 0.069±0.001 到 4.50±0.145 min-1,表现出广谱微量污染物降解能力。实验分析和动力学模型的证据表明,在 UVA-LED/PI AOP 中生成的主要物种是羟基自由基(OH)和臭氧(O),它们对 NPX 降解的贡献相当。增加 pH 值和辐照波长会对 NPX 的降解产生负面影响,这可以通过 PI 的量子产率(Φ)降低得到很好的解释。在水基质(即氯、碳酸氢盐和腐殖酸)和实际水样存在的情况下,考察了 UVA-LED/PI AOP 对 NPX 的降解动力学,并说明了潜在的机制。从 UVA-LED/PI AOP 氧化 NPX 中总共鉴定出 9 种转化产物,主要通过羟化、脱烷基和氧化途径。UVA-LED/PI AOP 可能是一种有前途的处理水溶液中微量污染物的技术。在 PI 的光解过程中,Φ 的关键作用可能会指导未来的光辅助 PI AOP 设计。