生物降解对聚乳酸微塑料吸附土霉素行为的影响

Effect of biodegradation on the adsorption behavior of oxytetracycline by polylactic acid microplastics

  • 摘要: 可降解塑料被评估为传统塑料的有前途的替代品。尽管微塑料被报道为环境中污染物的载体,但关于可降解微塑料在生物降解过程中吸附抗生素的行为与机制仍不明确。为了解环境中生物可降解微塑料对抗生素的吸附行为,开展了聚乳酸(PLA)微塑料在生物降解前后对土霉素(OTC)的吸附/解吸实验。结果表明:PLA在污水中自然降解35 d后,PLA表面形成致密的生物膜,酯类官能团特征峰红外强度降低,酯键断裂,发生了降解。根据Langmuir等温模型拟合结果,初始PLA对OTC的最大吸附能力为581.19 μg/g,生物膜的生成使PLA对OTC的吸附能力提高了20.15%,这主要是由于OTC与生物膜中的化学官能团(如N—H官能团)发生络合。脱除生物膜后,PLA表面暴露更多的含氧官能团,氢键作用增强,其对OTC的吸附量增加了39.01%。OTC在PLA上的吸附量随溶液初始pH的升高先增大后减小,富里酸显著抑制OTC在PLA表面的吸附,当富里酸浓度为200 mg/L时,PLA对OTC的吸附量减少了13.25%~61.79%。综上表明,生物降解增强了PLA对OTC的吸附,不利于水中抗生素的迁移转化,且抗生素通过微塑料在生物体内传播和积累,将增加生物体的生态风险。本研究通过揭示PLA在生物降解过程中对OTC的吸附行为,有助于了解可降解微塑料的环境吸附行为。

     

    Abstract: Biodegradable plastics have been evaluated as promising alternatives for conventional polymers in various fields. However, the adsorption behaviors and mechanisms of antibiotics onto biodegradable microplastics during their natural degradation remain poorly understood. To shed light on this issue, we conducted adsorption/desorption experiments on oxytetracycline (OTC) by polylactic acid (PLA) microplastics, comparing pre- and post-biodegradation conditions. The results showed that after 35 days of PLA natural degradation in wastewater, a dense biofilm formed on PLA surface, causing a decrease in the infrared intensity of ester functional group characteristic peak and suggesting bond rupture and degradation. The Langmuir isotherm model analysis revealed an initial adsorption capacity of 581.19 μg/g for OTC on PLA. The biofilm's presence increased the adsorption by 20.15%, primarily due to the complexation between OTC and biofilm's N—H functional groups. After biofilm removal, more oxygen-containing groups were exposed on the PLA's surface, enhancing hydrogen bonding and boosting OTC adsorption by 39.01%. The adsorption capacity of OTC on PLA increased first and then decreased with the increase of initial solution pH. Fulvic acid significantly influenced adsorption, reducing it by 13.25%-61.79% when presented at 200 mg/L. In summary, PLA's biodegradation enhances its OTC adsorption, potentially hindering antibiotic migration and transformation in water. This process highlights the ecological risk associated with microplastics carrying antibiotics, as they can accumulate in organisms. Revealing the OTC adsorption behavior of PLA during biodegradation contributes to a comprehensive understanding of degradable microplastics' environmental impact.

     

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