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利用物种特异性富集稳定同位素研究法国北部德勒河高污染沉积物中的汞甲基化和去甲基化作用。

Mercury methylation and demethylation in highly contaminated sediments from the Deûle River in Northern France using species-specific enriched stable isotopes.

作者信息

Ouddane Baghdad, Monperrus Mathilde, Kadlecova Milada, Daye Mirna, Amouroux David

机构信息

Université, Lille 1, Equipe de Physico-Chimie de l'Environnement, UMR CNRS LASIR 8516, Bat. C8 2°étage, 59655 Villeneuve d'Ascq Cedex, France.

出版信息

Environ Sci Process Impacts. 2015 Jan;17(1):145-55. doi: 10.1039/c4em00398e. Epub 2014 Nov 25.

Abstract

The methylation-demethylation processes in sediments of the Deûle River were determined using well-established isotope experiments. For this purpose, species-specific isotopically enriched tracers in the form of inorganic mercury IHg ((199)Hg) and methylmercury MeHg (Me(201)Hg) were used to determine Hg dynamics in the Deûle River. Sediment cores were collected at two sampling locations chosen in the most polluted zone of the Deûle River (Northern France) in proximity of a Zn, Pb, Cu, and Ni smelter called "Metaleurop" that had closed in 2003. Site I was chosen in the vicinity of the historic smelter site and site II upstream of the Deûle River. The incubation was realized directly in the sediment cores during the 24 hour experiment under environmental conditions close to the real natural systems (the same temperature, pH, humidity, light/dark conditions, oxygen levels…). The enriched isotopes were injected by needle into different sections of the core. After incubation, the core was sliced and the concentration of Hg species was determined in each section. The highest methylation potentials were found at sediment depths away from the sediment-water-interface. At site I, the methylation potential varied between 0.02-0.9% and at site II between 0.001-0.2%. The demethylation potentials fluctuated between 0.001-60% at site I and between 4-53% at site II. In both sites, negative net methylation potentials were obtained in several sediment depths, representing a net sink for MeHg. The average net methylation potential in site I demonstrated a negative value of 1919 ng g(-1) day(-1). It seems that in site I the demethylation process predominates methylation. Whereas, in site II, the average net methylation potential was a positive value of 138 ng g(-1) day(-1), demonstrating the dominance of methylation over demethylation.

摘要

利用成熟的同位素实验测定了德勒河沉积物中的甲基化-去甲基化过程。为此,使用无机汞IHg((199)Hg)和甲基汞MeHg(Me(201)Hg)形式的物种特异性同位素富集示踪剂来测定德勒河中的汞动态。在法国北部德勒河污染最严重区域内靠近一家名为“Metaleurop”的锌、铅、铜和镍冶炼厂(该冶炼厂已于2003年关闭)的两个采样点采集了沉积物岩芯。采样点I选在历史冶炼厂遗址附近,采样点II选在德勒河上游。在接近真实自然系统的环境条件(相同温度、pH值、湿度、光照/黑暗条件、氧气水平等)下,在24小时实验期间直接在沉积物岩芯中进行培养。通过针将富集的同位素注入岩芯的不同部分。培养后,将岩芯切片,并测定每个部分中汞物种的浓度。在远离沉积物-水界面的沉积物深度处发现了最高的甲基化潜力。在采样点I,甲基化潜力在0.02 - 0.9%之间变化,在采样点II在0.001 - 0.2%之间变化。去甲基化潜力在采样点I为0.001 - 60%之间波动,在采样点II为4 - 53%之间波动。在两个采样点的几个沉积物深度处都获得了负的净甲基化潜力,这代表了甲基汞的净汇。采样点I的平均净甲基化潜力显示为-1919 ng g(-1) 天(-1) 的负值。似乎在采样点I,去甲基化过程占甲基化的主导。而在采样点II,平均净甲基化潜力为138 ng g(-1) 天(-1) 的正值,表明甲基化优于去甲基化。

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