School of Environment, Hangzhou Institute for Advanced Study, UCAS, Hangzhou, Zhejiang 310024, China; State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.
State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China; College of Resources and Environment, University of Chinese Academy of Sciences, Beijing 100049, China.
Sci Total Environ. 2023 Oct 10;894:164928. doi: 10.1016/j.scitotenv.2023.164928. Epub 2023 Jun 20.
To fulfill the growing demand for retarding the oxidation of polymers and minimizing their migration from various products, new macromolecular synthetic phenolic antioxidants (SPAs) have emerged in the market. There is a concern that these SPAs may be released into wastewater streams during their manufacturing and use, eventually ending up in wastewater treatment plants (WWTPs). Nevertheless, information regarding the occurrence of these SPAs in sludge, particularly on a national scale, is scarce. In this study, several macromolecular SPAs and their transformation products (TPs) were investigated in sludge samples from 45 Chinese municipal WWTPs. All 14 analytes were detected in the sludge samples, among which, 12 analytes were first reported in sludge. 2,4,6-tri-tert-butylphenol (AO246) and 2 macromolecular SPAs, pentaerythritol tetrakis[3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate] (AO1010) and octadecyl-3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate (AO1076), were the most dominant SPAs, with geometric mean (GM) concentrations of 547, 212, and 35.2 ng/g dw, respectively. Two TPs, 3-(3,5-di-tert-butyl-4-hydroxyphenyl)propanoic acid (fenozan) and 3,5-di-tert-butyl-4-hydroxybenzoic acid (BHT-COOH), were found in some sludge samples (48.9-71.1 %) with GM of 45.5 and 12.8 ng/g dw, respectively. By using LC-Q-TOF-MS/MS analysis, we tentatively identified previously unknown TPs of 10 macromolecular SPAs in sludge. This suggests that there are still unclear mechanisms modulating the transformation of these SPAs, which underscores the complexity of their fate. Additionally, using the freshwater photobacteria Vibrio qinghaiensis sp.-Q67 (Q67) as model organism, the acute and chronic EC of the 14 analytes were assessed for ecological risk assessment. By considering toxicity data obtained from algae, daphnia, and fish collected or predicted from various databases, we found that these analytes, including their mixture at low detected concentrations, pose risks to aquatic systems that should not be disregarded. Overall, the current study provides a comprehensive overview of novel SPAs and their TPs in sludge, offering valuable insights for investigating their environmental behavior, fate, and risks.
为了满足聚合物抗氧化和最小化其从各种产品中迁移的需求不断增长，市场上出现了新的高分子合成酚类抗氧化剂（SPAs）。人们担心这些 SPA 在制造和使用过程中可能会释放到废水中，最终进入废水处理厂（WWTP）。然而，关于这些 SPA 在污泥中的存在情况，特别是在全国范围内的信息却很少。在这项研究中，研究人员调查了来自中国 45 个城市 WWTP 的污泥样本中的几种高分子 SPA 和它们的转化产物（TPs）。所有 14 种分析物都在污泥样本中被检测到，其中 12 种分析物是首次在污泥中被报道。2,4,6-三-叔丁基苯酚（AO246）和 2 种高分子 SPA，季戊四醇四[3-(3,5-二叔丁基-4-羟基苯基)丙酸酯]（AO1010）和十八烷基-3-(3,5-二叔丁基-4-羟基苯基)丙酸酯（AO1076）是最主要的 SPA，几何平均值（GM）浓度分别为 547、212 和 35.2ng/g dw。两种 TPs，3-(3,5-二叔丁基-4-羟基苯基)丙酸（fenozan）和 3,5-二叔丁基-4-羟基苯甲酸（BHT-COOH）在一些污泥样本中被发现（48.9-71.1%），其 GM 分别为 45.5 和 12.8ng/g dw。通过使用 LC-Q-TOF-MS/MS 分析，我们初步鉴定了污泥中 10 种高分子 SPA 的未知 TPs。这表明仍然存在不清楚的机制来调节这些 SPA 的转化，这突显了它们命运的复杂性。此外，研究人员还使用淡水发光菌青海弧菌 Q67（Q67）作为模型生物，评估了 14 种分析物的急性和慢性 EC，用于生态风险评估。通过考虑从藻类、水蚤和鱼类中获得的毒性数据，以及从各种数据库中收集或预测的数据，研究人员发现这些分析物，包括在低检测浓度下的混合物，对水生系统构成了风险，不容忽视。总的来说，本研究全面概述了污泥中的新型 SPA 和它们的 TPs，为研究它们的环境行为、命运和风险提供了有价值的见解。
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