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Analyzing (Initial) Biotransformation Reactions as an Organizing Principle for Unraveling the Extent of Trace Organic Chemical Biotransformation in Biofiltration Systems
ACS ES&T Water ( IF 4.8 ) Pub Date : 2021-07-15 , DOI: 10.1021/acsestwater.1c00145
Uwe Hübner 1 , David Wolff 2 , Stefan Achermann 3 , Jörg E. Drewes 1 , Arne Wick 2 , Kathrin Fenner 3, 4
Affiliation  

Due to the low environmental concentrations and substance-specific behavior of trace organic chemicals (TOrCs), general mechanistic insights can hardly be gained from biotransformation studies with individual substances. In this study, we aimed to identify prevalent enzymatic reactions under different redox and substrate conditions in a well-defined laboratory-scale column system. Biotransformation of chemicals in the first column, which was characterized by a relatively high biomass and rapid depletion of dissolved oxygen, was initiated by frequent and fast reactions such as the oxidation of alcohols or amide hydrolysis. Slower reactions, e.g., the initial dealkylation of primary and secondary amines, were inefficient in the first column and benefited from oxic and carbon-limited conditions prevalent in the second column system after reaeration. Moreover, several compound-specific reactions such as the cleavage of C–Cl and C–O bonds through substitution with glutathione occurred only under carbon-limited conditions. The link between system-specific TOrC removal and suggested initial reactions from the literature can serve as a starting point for a suspect screening of relevant enzymes for the biotransformation of TOrCs based on metagenomic or metatranscriptomic data. Complementary batch experiments with media from the columns confirmed the observed removal under carbon-rich conditions but revealed a limited reproducibility of microbial degradation under oligotrophic conditions.

中文翻译:

分析(初始)生物转化反应作为揭示生物过滤系统中痕量有机化学生物转化程度的组织原则

由于微量有机化学物质 (TOrC) 的环境浓度低和物质特定行为,因此很难从单个物质的生物转化研究中获得一般的机制见解。在本研究中,我们的目标是在定义明确的实验室规模柱系统中,确定不同氧化还原和底物条件下普遍存在的酶促反应。第一列中化学品的生物转化,其特点是生物量相对较高,溶解氧迅速消耗,是由频繁和快速的反应引发的,例如醇的氧化或酰胺水解。较慢的反应,例如伯胺和仲胺的初始脱烷基,在第一个塔中效率低下,并且受益于再充气后第二个塔系统中普遍存在的含氧和碳限制条件。此外,一些化合物特异性反应,例如通过用谷胱甘肽取代而裂解 C-Cl 和 C-O 键,仅在碳限制条件下发生。系统特异性 TOrC 去除与文献中建议的初始反应之间的联系可以作为基于宏基因组或宏转录组数据对 TOrC 生物转化相关酶进行可疑筛选的起点。用柱子中的介质进行的补充批次实验证实了在富碳条件下观察到的去除,但揭示了在贫营养条件下微生物降解的重现性有限。系统特异性 TOrC 去除与文献中建议的初始反应之间的联系可以作为基于宏基因组或宏转录组数据对 TOrC 生物转化相关酶进行可疑筛选的起点。用柱子中的介质进行的补充批次实验证实了在富碳条件下观察到的去除,但揭示了在贫营养条件下微生物降解的重现性有限。系统特异性 TOrC 去除与文献中建议的初始反应之间的联系可以作为基于宏基因组或宏转录组数据对 TOrC 生物转化相关酶进行可疑筛选的起点。用柱子中的介质进行的补充批次实验证实了在富碳条件下观察到的去除,但揭示了在贫营养条件下微生物降解的重现性有限。
更新日期:2021-08-13
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