School of Environment, Guangdong Key Laboratory of Environmental Pollution and Health, Jinan University, Guangzhou, 510632, China.
Chemosphere. 2022 Sep;303(Pt 1):134968. doi: 10.1016/j.chemosphere.2022.134968. Epub 2022 May 14.
Remdesivir (RDV), dexamethasone (DEX) and hydroxychloroquine (HCQ) were widely used in the treatment of COVID-19 pneumonia, possibly causing environmental risks and drug-resistance viruses. This study elucidated the degradation mechanisms and potential toxicity risks of the three anti-COVID-19 drugs by UV and ultraviolet-coupled advanced oxidation processes (UV/AOPs). All the drugs could be degraded by more than 98% within 3 min under the following optimal conditions: pH of 5.0 and drug-to-oxidant (HO) molar ratio of 1:200. Combined with density functional theory (DFT) analysis and high-performance liquid chromatography quadrupole time-of-flight mass spectrometry (HPLC-QTOF-MS), twenty-four transformation products (TPs) were detected and the main degradation pathways were investigated. Based on bacterial luminescence inhibition test and the peak-area evolution of TPs, RDV and HCQ showed an obvious toxicity-increase region when TPs were generated in large quantities, while the toxicity of DEX continued to decline during degradation processes. By QSAR predictions, the main contributors to the toxicity evolution during the UV/AOPs were predicted. Halogen-containing TPs showed significantly higher toxicity than other TPs, and thus the chlorine-containing structure in HCQ presented the potential toxicity. Appropriate reaction parameters and adequate reaction time for the UV/AOPs could eliminate the toxicity of TPs and ensure environmental safety. This study could play a positive role in the treatment of anti-COVID-19 drugs and their environmental hazard assessment.
瑞德西韦（RDV）、地塞米松（DEX）和羟氯喹（HCQ）在治疗 COVID-19 肺炎中被广泛应用，可能会造成环境风险和耐药病毒。本研究通过紫外线和紫外线耦合高级氧化工艺（UV/AOPs）阐明了这三种抗 COVID-19 药物的降解机制和潜在毒性风险。在以下最佳条件下，所有药物在 3 分钟内的降解率均超过 98%：pH 值为 5.0，药物与氧化剂（HO）的摩尔比为 1:200。结合密度泛函理论（DFT）分析和高效液相色谱四极杆飞行时间质谱（HPLC-QTOF-MS），检测到二十四个转化产物（TPs），并研究了主要的降解途径。基于细菌发光抑制试验和 TPs 的峰面积演变，当大量生成 TPs 时，RDV 和 HCQ 表现出明显的毒性增加区域，而 DEX 的毒性在降解过程中持续下降。通过定量构效关系（QSAR）预测，预测了在 UV/AOPs 过程中导致毒性演变的主要因素。含卤素的 TPs 表现出明显高于其他 TPs 的毒性，因此 HCQ 中的含氯结构表现出潜在的毒性。适当的反应参数和充足的反应时间对于 UV/AOPs 可以消除 TPs 的毒性并确保环境安全。本研究可以在治疗抗 COVID-19 药物及其环境危害评估方面发挥积极作用。
