Synergistic effects of fluorinated substituents and Fe(Ⅱ) on ferrihydrite transformation and antibiotic degradation

IF 6.2 2区环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES

Ecotoxicology and Environmental Safety Pub Date : 2025-05-17 DOI:10.1016/j.ecoenv.2025.118313

Liting Wang , Shikun Wei , Liwen Zhang , Zhiyong Guo , Yan Lei , Deming Dong

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引用次数: 0

Abstract

Ferrihydrite is commonly associated with antibiotics in natural environments due to its strong sorption capabilities and high specific surface area. Under reducing conditions, Fe(II) acts as a catalyst for the transformation of ferrihydrite into more crystalline minerals. However, the influence of antibiotic molecular structure on the Fe(II)-catalyzed transformation of ferrihydrite and the associated degradation mechanisms of antibiotics have remained unclear. This study employed enoxacin (ENO), a representative fluorinated pharmaceutical, and pipemidic acid (PPA), a structural analog of ENO, to investigate the effect of fluorinated substituents on Fe(II)-facilitated ferrihydrite transformation. The results revealed that the transformation of ferrihydrite in the ENO system was 2.8 times greater than in the PPA system. ENO degradation reached 74.3 %, which was 1.13 times higher than that of PPA. ENO degradation products were more prone to hydroxylation, decarboxylation, and piperazine ring oxidation, whereas PPA degradation primarily involved oxidation of the piperazine ring. The fluorinated substituent in ENO facilitated ferrihydrite transformation by influencing the concentration of adsorbed Fe(II) and the distribution of antibiotics within the mineral inside. Furthermore, the fluorinated substituent in ENO enhanced degradation by increasing electron transfer between ENO and Fe(III), raising the content of adsorbed Fe(II) and promoting the formation of goethite. Collectively, these findings provide new insights into the environmental behavior of ferrihydrite and the fate of structurally different antibiotics in natural systems.

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氟化取代基与铁（Ⅱ）对水合铁转化和抗生素降解的协同效应

水合铁由于其强大的吸附能力和高比表面积，在自然环境中通常与抗生素有关。在还原条件下，铁（II）作为催化剂将水合铁转化为更多的结晶矿物。然而，抗生素分子结构对铁（II）催化水合铁转化及抗生素降解机制的影响尚不清楚。本研究采用代表性的氟化药物依诺沙星（ENO）和ENO的结构类似物哌啶酸（PPA），研究了氟化取代基对Fe（II）促进的水合铁转化的影响。结果表明，ENO体系中水合铁的转化率是PPA体系的2.8倍。ENO的降解率达到74.3 %，是PPA的1.13倍。ENO降解产物更倾向于羟基化、脱羧和哌嗪环氧化，而PPA降解主要涉及哌嗪环的氧化。ENO中的氟化取代基通过影响矿物内部吸附铁（II）的浓度和抗生素的分布，促进了水合铁的转化。此外，ENO中的氟化取代基通过增加ENO与Fe（III）之间的电子转移，提高吸附Fe（II）的含量，促进针铁矿的形成，从而增强了降解。总的来说，这些发现为水合铁的环境行为和自然系统中结构不同的抗生素的命运提供了新的见解。

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来源期刊

Ecotoxicology and Environmental Safety 环境科学-毒理学

CiteScore

12.10

自引率

5.90%

发文量

1234

审稿时长

88 days

期刊介绍： Ecotoxicology and Environmental Safety is a multi-disciplinary journal that focuses on understanding the exposure and effects of environmental contamination on organisms including human health. The scope of the journal covers three main themes. The topics within these themes, indicated below, include (but are not limited to) the following: Ecotoxicology、Environmental Chemistry、Environmental Safety etc.