Novel organophosphate esters and their transformation products in offshore sediment from Eastern China: Occurrence, temporal trend, and risk assessment

IF 10.3 1区环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES

Environment International Pub Date : 2025-01-01 DOI:10.1016/j.envint.2024.109205

Meng Gao , Yu Wang , Liman Wei , Siyuan Li , Qiuyue Zhang , Zhongkang Yang , Mohan Bai , Yiming Yao , Lei Wang , Hongwen Sun

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引用次数: 0

Abstract

Offshore sediment serves as an important sink for traditional organophosphate esters (TOPEs) originating from terrestrial sources. However, the contamination characteristics of novel OPEs (NOPEs) and their hydrolyzed and hydroxylated transformation products (Di- and OH-OPEs) in marine sediment are still unknown. In this study, 34 OPE-associated contaminants were measured in six offshore sediment cores (71 samples) collected from Eastern China. The total concentrations of Σ₁₅TOPEs, Σ₃NOPEs, Σ₉Di-OPEs, and Σ₇OH-OPEs in surface sediments were 3.16–73.4, n.d.–16.3, 4.48–21.4, and 0.14–0.42 ng g⁻¹, respectively. NOPE compounds, such as tris(2,4-di-tert-butylphenyl) phosphate and its diester product, exhibited high contamination levels, primarily due to their high hydrophobicity and extensive industrial applications. Additionally, atmospheric transportation, along with wet and dry deposition and ocean currents, plays a crucial role in their distribution in offshore sediment. The location conditions and historical usage also influenced the vertical distributions of OPE-associated contaminants in sediment cores. Notably, a concentration peak of bis(2,4-di-tert-butylphenyl) phosphate (B2,4DtBPP) was dating back to 1940s, indicating the early usage of antioxidant tris(2,4-di-tert-butylphenyl) phosphite. Furthermore, a risk quotient (RQ) model was employed to assess the ecological risks posed by OPEs. Generally, the acute toxicity-based predicted no-effect concentrations for studied compounds were 1 to 2 orders of magnitude lower than those based on chronic toxicity. NOPEs and B2,4DtBPP exhibited high ecological risks, with maximum RQ values of 1570–4877 based on acute toxicity and 93.4–197 based on chronic toxicity. Notably, ΣRQ values for NOPEs were significantly higher than those of TOPEs (Mann-Whitney U test, p < 0.001), indicating their severe ecological risks in offshore sediment. Therefore, given the continuous input and considerable persistence of NOPEs in offshore sediment, their toxic effects and mechanisms warrant thorough investigation. This study provides the first evidence for the occurrence, temporal trends, and potential risks of NOPEs in marine sediment environment.

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中国东部近海沉积物中新型有机磷酯及其转化产物：发生、时间趋势及风险评价

近海沉积物是源自陆地的传统有机磷酸酯（TOPEs）的重要汇。然而，新型OPEs （NOPEs）及其水解和羟基化转化产物（Di-和OH-OPEs）在海洋沉积物中的污染特性尚不清楚。本研究在中国东部海域采集的6个近海沉积物岩心（71个样品）中测量了34种与ope相关的污染物。表层沉积物中Σ15TOPEs、Σ3NOPEs、Σ9Di-OPEs和Σ7OH-OPEs的总浓度分别为3.16 ~ 73.4、4.48 ~ 21.4和0.14 ~ 0.42 ng/g。NOPE化合物，如三（2,4-二叔丁基苯基）磷酸盐及其二酯产品，表现出高污染水平，主要是由于它们的高疏水性和广泛的工业应用。此外，大气运输、干湿沉积和洋流对其在近海沉积物中的分布起着至关重要的作用。位置条件和历史使用对沉积物岩心中ope相关污染物的垂直分布也有影响。值得注意的是，二（2,4-二叔丁基苯基）磷酸（B2,4DtBPP）的浓度峰值可以追溯到1940年 s，这表明抗氧化剂三（2,4-二叔丁基苯基）亚磷酸酯的早期使用。在此基础上，采用风险商（RQ）模型对露天采场的生态风险进行了评价。一般来说，研究化合物的急性毒性预测无效应浓度比基于慢性毒性的预测浓度低1到2个数量级。NOPEs和B2、4DtBPP具有较高的生态风险，急性毒性RQ值最高为1570 ~ 4877，慢性毒性RQ值最高为93.4 ~ 197。值得注意的是，NOPEs的ΣRQ值显著高于TOPEs (Mann-Whitney U检验，p <； 0.001)，表明NOPEs在近海沉积物中的生态风险较大。因此，考虑到近海沉积物中NOPEs的持续输入和相当长的持久性，它们的毒性效应和机制值得深入研究。本研究首次揭示了海洋沉积物环境中NOPEs的发生、时间趋势和潜在风险。

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来源期刊

Environment International 环境科学-环境科学

CiteScore

21.90

自引率

3.40%

发文量

734

审稿时长

2.8 months

期刊介绍： Environmental Health publishes manuscripts focusing on critical aspects of environmental and occupational medicine, including studies in toxicology and epidemiology, to illuminate the human health implications of exposure to environmental hazards. The journal adopts an open-access model and practices open peer review. It caters to scientists and practitioners across all environmental science domains, directly or indirectly impacting human health and well-being. With a commitment to enhancing the prevention of environmentally-related health risks, Environmental Health serves as a public health journal for the community and scientists engaged in matters of public health significance concerning the environment.