PowerChina Zhongnan Engineering Corporation Limited, Changsha 410004, China.
Hunan First Normal University, Changsha 410114, China.
Int J Environ Res Public Health. 2022 Sep 28;19(19):12354. doi: 10.3390/ijerph191912354.
Advanced oxidation technology represented by hydroxyl radicals has great potential to remove residual antibiotics. In this study, we systematically compared the metronidazole (MTZ) degradation behavior and mechanism in the UV and UV/HO systems at pH 3.00 condition. The results show that the initial reaction rates were 0.147 and 1.47 µM min in the UV and UV/HO systems, respectively. The main reason for the slow direct photolysis of MTZ is the relatively low molar absorption coefficient (2645.44 M cm) and quantum yield (5.9 × 10 mol Einstein). Then, we measured kMTZ,OH • as 2.79 (±0.12) × 10 M s by competitive kinetics, and calculated kMTZ,OH • and [OH •]SS as 2.43 (±0.11) × 10 M s and 2.36 × 10 M by establishing a kinetic model based on the steady-state hypothesis in our UV/HO system. The contribution of direct photolysis and OH to the MTZ degradation was 9.9% and 90.1%. OH plays a major role in the MTZ degradation, and OH was the main active material in the UV/HO system. This result was also confirmed by MTZ degradation and radicals' identification experiments. MTZ degradation increases with HO dosage, but excessive HO had the opposite effect. A complex matrix has influence on MTZ degradation. Organic matter could inhibit the degradation of MTZ, and the quenching of the radical was the main reason. NO3- promoted the MTZ degradation, while SO42- and Cl had no effect. These results are of fundamental and practical importance in understanding the MTZ degradation, and to help select preferred processes for the optimal removal of antibiotics in natural water bodies, such as rivers, lakes, and groundwater.
高级氧化技术以羟基自由基为代表,具有去除残留抗生素的巨大潜力。本研究在 pH 3.00 条件下,系统比较了紫外光和紫外/HO 体系中甲硝唑(MTZ)的降解行为和机制。结果表明,紫外光和紫外/HO 体系中的初始反应速率分别为 0.147 和 1.47 μM min。MTZ 直接光解缓慢的主要原因是其摩尔吸收系数(2645.44 M cm)和量子产率(5.9×10 mol Einstein)较低。然后,我们通过竞争动力学测量得到 kMTZ,OH·为 2.79(±0.12)×10 M s,并通过在我们的紫外/HO 体系中基于稳态假设建立动力学模型,计算得到 kMTZ,OH·和[OH·]SS 分别为 2.43(±0.11)×10 M s 和 2.36×10 M。紫外光和 HO 对 MTZ 降解的贡献分别为 9.9%和 90.1%。OH 在 MTZ 降解中起主要作用,OH 是紫外/HO 体系中的主要活性物质。这一结果也得到了 MTZ 降解和自由基鉴定实验的证实。随着 HO 剂量的增加,MTZ 的降解增加,但过量的 HO 则产生相反的效果。复杂基质对 MTZ 降解有影响。有机物可以抑制 MTZ 的降解,自由基猝灭是主要原因。NO3-促进了 MTZ 的降解,而 SO42-和 Cl-则没有影响。这些结果对于理解 MTZ 的降解以及帮助选择去除天然水体(如河流、湖泊和地下水)中抗生素的首选工艺具有重要的理论和实际意义。