College of Resources and Environment, Shanxi University of Finance and Economics, Taiyuan, 030006, China; Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Institute of Atmospheric Sciences, Department of Environmental Science and Engineering, Fudan University, Shanghai, 200433, China.
College of Marine Ecology and Environment, Shanghai Ocean University, Shanghai, 201306, China.
Chemosphere. 2021 Jan;263:128100. doi: 10.1016/j.chemosphere.2020.128100. Epub 2020 Aug 27.
We reconstructed the history of the inputs of hexachlorocyclohexanes (HCHs) and dichlorodiphenyltrichloroethanes (DDTs) into the marine environment to reveal the time-dependent influence of sources and associated anthropogenic activities in China, based on Pb-dated cores from the East China marginal seas (ECMS). The temporal dynamics of pesticide contamination expresses as deposition fluxes, inventories, and half-life estimations varied among the cores, suggesting heterogeneity in transport pathways of pollutants. The depth profiles of pesticide inputs closely followed their historical production and application timelines in China, and were also affected by human activities in catchments, with general declines in HCH and DDT inputs to the coring sites after their peak deposition. Despite the prevalence of occurrence of weathered HCH/DDT in the cores, there were clear source-dependent differences in isomeric composition and accumulation between before and after these pesticides were banned. α-HCH and p,p'-DDT were relatively more enriched in sediments from the pre-ban period when heavy technical HCHs and DDTs use occurred, as indicated by the higher α-/β-HCH and lower (DDE + DDD)/DDTs ratios, and the larger fractions of α-HCH and p,p'-DDT influxes to the coring sites in the ΣHCH and ΣDDT fluxes, respectively, while this pattern shifted to be historical residue-based in the post-ban period. The difference in the recent influxes of pesticides to core sediments and their higher post-ban inventories highlight the increasing importance of historical sources over time and continuous input of weathered residues into marine environment via lateral transport.
我们重建了六氯环己烷(HCHs)和滴滴涕(DDTs)输入海洋环境的历史,以揭示中国来源和相关人为活动随时间的变化对其的影响,该研究基于来自中国东海边缘海(ECMS)的 Pb 年代测年岩芯。农药污染的时间动态表现为沉积通量、储量和半衰期估计值在各岩芯之间存在差异,表明污染物的传输途径存在异质性。农药输入的深度剖面与中国历史上的生产和应用时间线密切相关,也受到集水区人类活动的影响,在这些农药的沉积高峰期过后,其输入到岩芯地点的量普遍下降。尽管在岩芯中普遍存在风化的 HCH/DDT,但在这些农药被禁用前后,其同系物组成和积累仍存在明显的来源依赖性差异。α-HCH 和 p,p'-DDT 在禁用前时期的沉积物中相对更为富集,这表明在大量使用技术 HCHs 和 DDTs 时,α-/β-HCH 比值较高,(DDE + DDD)/DDTs 比值较低,以及在ΣHCH 和 ΣDDT 通量中,α-HCH 和 p,p'-DDT 分别向岩芯输入的通量较大,而在禁用后时期,这种模式转变为基于历史残留的模式。农药对岩芯沉积物最近的输入通量的差异及其在禁用后更高的储量突出了随着时间的推移历史来源的重要性不断增加,以及风化残留物通过侧向传输不断输入海洋环境。