Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, College of Environment & Ecology, Chongqing University, Chongqing, 400045, China.
Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, College of Environment & Ecology, Chongqing University, Chongqing, 400045, China.
Chemosphere. 2021 Nov;282:131115. doi: 10.1016/j.chemosphere.2021.131115. Epub 2021 Jun 7.
Pharmaceuticals may pose serious potential risks, such as biological responses and chronic health effects, due to their ubiquitous in natural aquatic water bodies. In this study, we proposed an effective, feasible, and low-cost strategy for the abatement of pharmaceuticals (i.e., phenylbutazone (PBZ) and sulfinpyrazone (SPZ)) via CoO nanoparticles (NPs) as heterogeneous catalyst in permanganate (Mn(VII)) oxidation for the first time. The performance of the CoO NPs in permanganate oxidation is highly dependent on pH and its dosage. CoO NPs play as electron shuttles in the catalytic permanganate oxidation process involving one-electron transfer with the oxidation of ≡Co to ≡Co by permanganate and the formation of colloidal manganese dioxide (MnO), as well as the reduction of the newly formed ≡Co to ≡Co by organics and the production of oxidized organic byproducts. The degradation pathways of PBZ and SPZ in catalytic permanganate oxidation were proposed based on the liquid chromatography-tandem mass spectrometry (LC-MS/MS) results and Gaussian calculation, and the toxicity decay of pharmaceuticals during oxidation was observed. Considering the stability, reusability, and cost, CoO coupled with Mn(VII) is suitable for water pretreatment and is potentially feasible for industrial application, which is not only effective for decomposing PBZ and SPZ, but also for eliminating their toxicity.
由于药品在天然水生水体中的普遍存在,它们可能会带来严重的潜在风险,如生物反应和慢性健康影响。在这项研究中,我们首次提出了一种有效、可行且低成本的策略,通过 CoO 纳米粒子 (NPs) 作为多相催化剂,在高锰酸盐 (Mn(VII)) 氧化中去除药品(即苯丁唑酮 (PBZ) 和磺吡唑酮 (SPZ))。CoO NPs 在高锰酸盐氧化中的性能高度依赖于 pH 值及其用量。在涉及单电子转移的催化高锰酸盐氧化过程中,CoO NPs 作为电子穿梭体发挥作用,其中高锰酸盐将 ≡Co 氧化为 ≡Co,并形成胶体二氧化锰 (MnO),同时新形成的 ≡Co 被有机物还原,并产生氧化的有机副产物。基于液质联用 (LC-MS/MS) 结果和高斯计算,提出了 PBZ 和 SPZ 在催化高锰酸盐氧化中的降解途径,并观察了药品在氧化过程中的毒性衰减。考虑到稳定性、可重复使用性和成本,CoO 与 Mn(VII) 结合适合用于水的预处理,并且具有潜在的工业应用可行性,不仅有效地分解了 PBZ 和 SPZ,还消除了它们的毒性。