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Analysis of the aerobic biodegradation of glucocorticoids: Elucidation of the kinetics and transformation reactions.
Water Research ( IF 11.4 ) Pub Date : 2020-01-30 , DOI: 10.1016/j.watres.2020.115561
Alexander Weizel 1 , Michael P Schlüsener 1 , Georg Dierkes 1 , Arne Wick 1 , Thomas A Ternes 1
Affiliation  

Glucocorticoids (GCs) are one of the most prescribed pharmaceutical classes worldwide. They have reached the focus as environmental pollutants in the current scientific research, due to their potential risks to aquatic organisms even in the lower ng L-1 range. The objective of this study was to determine the kinetic behavior of selected GCs and to identify their main transformation products (TPs) in lab scaled biodegradation experiments. Therefore, we analyzed the removal of 13 GCs in aerated incubation experiments with activated sludge taken from a German municipal wastewater treatment plant (WWTP) as inoculum. For all steroids, an exponential decrease of the concentrations was observed, which was modelled by pseudo-first order kinetics. Overall, the rate constants kbiol. ranged from 0.07 L gss-1 d-1 (triamcinolone acetonide) to 250 L gss-1 d-1 (prednisolone). These results emphasize the broad variation in the biodegradability and recalcitrance of certain GCs. The selection of the studied GCs enabled a deduction of microbiological stability related to functional groups. Based on the identified TPs, a variety of enzymatically mediated reactions were postulated. Moreover, the identified TPs are characterized by an intact steroid core structure. Thus residual endocrine activity cannot be ruled out. The main observed reactions were regioselective hydrogenation of carbon double-bonds, degradation of the steroid C17 side-chain, ester hydrolysis and oxidative hydroxylation. In total, 41 TPs were tentatively identified and 22 of them were unambiguously confirmed via reference standards. Additionally, 12 TPs were detected in the effluents of municipal WWTPs and, to the best of our knowledge, the occurrence of eight of these TPs has been shown for the first time. These TPs might significantly contribute to the detected residual endocrine activities in the aquatic environments. Therefore, there is a strong need for efficient removal strategies, in particular for persistent steroid hormones with elevated potencies.

中文翻译:

糖皮质激素的有氧生物降解分析:动力学和转化反应的阐明。

糖皮质激素(GCs)是全球处方最广泛的药物类别之一。由于它们对水生生物甚至在ng L-1范围以下的潜在风险,它们已成为当前科学研究中环境污染物的焦点。这项研究的目的是确定所选GC的动力学行为,并在实验室规模的生物降解实验中确定其主要转化产物(TP)。因此,我们在曝气温育实验中分析了13种GC的去除情况,这些实验采用的活性污泥取自德国市政废水处理厂(WWTP)作为接种物。对于所有类固醇,均观察到浓度呈指数下降,这是通过拟一级动力学建模的。总体而言,速率常数kbiol。范围从0。07 L gss-1 d-1(曲安奈德)至250 L gss-1 d-1(泼尼松龙)。这些结果强调了某些气相色谱仪在生物降解性和难降解性方面的广泛差异。对所研究的GC的选择使得能够推断出与官能团有关的微生物稳定性。基于已鉴定的TP,推测了多种酶促反应。而且,所鉴定的TPs以完整的类固醇核心结构为特征。因此,不能排除残留的内分泌活性。观察到的主要反应是碳双键的区域选择性氢化,类固醇C17侧链的降解,酯水解和氧化羟基化。初步确定了41种TP,通过参考标准明确确定了22种。另外,据我们所知,在市政污水处理厂的废水中检测到了12种TP,据我们所知,这是首次发现了其中8种TP。这些TP可能对水生环境中检测到的残留内分泌活动有重要贡献。因此,强烈需要有效的去除策略,尤其是对于具有增强效力的持久性类固醇激素。
更新日期:2020-01-31
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