Abstract：
β-lactam antibiotics, extensively used worldwide, pose significant risks to human health and ecological safety due to their accumulation in the environment. Recent studies have demonstrated the efficacy of transition metal-activated sulfite systems, like Fe(Ⅲ)/HSO3-, in removing PPCPs from water. However, research on their capability to degrade β-lactam antibiotics remains sparse. This paper evaluates the degradation of 14 types of β-lactam antibiotics in Fe(Ⅲ)/HSO3- system and establishes a QSAR model correlating molecular descriptors with degradation rates using the MLR method. Using cefazolin as a case study, this research predicts degradation pathways through NPA charge and Fukui function analysis, corroborated by UPLC-MS product analysis. The investigation further explores the influence of variables such as HSO3- dosage, substrate concentration, Fe(Ⅲ) dosage, initial pH and the presence of common seen water matrices including humic acid and bicarbonate on the degradation efficiency. Optimal conditions for cefazolin degradation in Fe(Ⅲ)/HSO3- system were determined to be 93.3 μM HSO3-, 8.12 μM Fe(Ⅲ) and an initial pH of 3.61, under which the interaction of Fe(Ⅲ) dosage with initial pH was found to significantly affect the degradation efficiency. This study not only provides a novel degradation approach for β-lactam antibiotics but also expands the theoretical application horizon of the Fe(Ⅲ)/HSO3- system.
摘要：
β-内酰胺类抗生素,在世界范围内广泛使用，由于它们在环境中的积累，对人类健康和生态安全构成重大风险。最近的研究已经证明了过渡金属活化亚硫酸盐系统的功效，如Fe(Ⅲ)/HSO3-，从水中去除PPCPs。然而,关于它们降解β-内酰胺类抗生素的能力的研究仍然很少。本文评价了14种β-内酰胺类抗生素在Fe(Ⅲ)/HSO3-体系中的降解情况,并利用MLR方法建立了分子描述符与降解速率相关的QSAR模型。以头孢唑啉为例，这项研究通过NPA电荷和福井功能分析预测降解途径，UPLC-MS产品分析证实。调查进一步探讨了HSO3-剂量等变量的影响，底物浓度,Fe(Ⅲ)用量,初始pH值和常见的水基质的存在，包括腐殖酸和碳酸氢盐对降解效率的影响。确定头孢唑啉在Fe（Ⅲ）/HSO3-体系中降解的最佳条件为93.3μMHSO3-，8.12μMFe（Ⅲ）和3.61的初始pH值，在此条件下，Fe（Ⅲ）的用量与初始pH值的相互作用显着影响降解效率。本研究不仅为β-内酰胺类抗生素的降解提供了新的途径,而且拓展了Fe(Ⅲ)/HSO3-体系的理论应用范围。
