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哈特韦尔湖超级基金场地多氯联苯污染沉积物的长期恢复:多氯联苯脱氯。2. 速率和程度。

Long-term recovery of PCB-contaminated sediments at the Lake Hartwell superfund site: PCB dechlorination. 2. Rates and extent.

作者信息

Magar Victor S, Brenner Richard C, Johnson Glenn W, Quensen John F

机构信息

Battelle Memorial Institute, 505 King Avenue, Columbus, Ohio 43201, USA.

出版信息

Environ Sci Technol. 2005 May 15;39(10):3548-54. doi: 10.1021/es0486216.

Abstract

This paper reports on extensive polychlorinated biphenyl (PCB) dechlorination measured in Lake Hartwell (Pickens County, SC) sediments. Vertical sediment cores were collected from 18 locations in Lake Hartwell (Pickens County, SC) and analyzed in 5-cm increments for PCB congeners. The preferential loss of meta and para chlorines with sediment depth demonstrated that PCBs in the sediments underwent reductive dechlorination after burial. Notably, ortho chlorines were highly conserved for more than 5 decades; since the first appearance of PCBs, ca. 1950-1955. These dechlorination characteristics resulted in the accumulation of lower chlorinated congeners dominated by ortho chlorine substituents. Dechlorination rates were determined by plotting the numbers of meta plus para chlorines per biphenyl molecule (mol of chlorine/mol of PCB) with sediment age. Regression analyses showed linear correlations between meta plus para chlorine concentrations with time. The average dechlorination rate was 0.094 +/- 0.063 mol of Cl/mol of PCB/yr. The rates measured using the 2001 cores were approximately twice those measured using the 2000 cores, most likely because the 2001 cores were collected only at transects O, L, and I, which had the highest rates measured in 2000. An inverse of the dechlorination rates indicated that 16.4 +/- 11.6 yr was required per meta plus para chlorine removal (ranging from 4.3 to 43.5 yr per chlorine removal). The rates determined from this study were 1-2 orders of magnitude lower than rates reported from laboratory microcosm studies using Hudson River and St. Lawrence River sediments, suggesting that dechlorination rates reported for laboratory experiments are much higher than those occurring in situ.

摘要

本文报道了在哈特韦尔湖(南卡罗来纳州皮肯斯县)沉积物中测得的多氯联苯(PCB)大量脱氯情况。从哈特韦尔湖(南卡罗来纳州皮肯斯县)的18个地点采集了垂直沉积物岩芯,并以5厘米的增量对多氯联苯同系物进行了分析。随着沉积物深度增加,间位和对位氯优先损失,这表明沉积物中的多氯联苯在埋藏后经历了还原脱氯。值得注意的是,邻位氯在50多年里高度保守;自多氯联苯首次出现以来,大约在1950 - 1955年。这些脱氯特征导致了以邻位氯取代基为主的低氯代同系物的积累。通过绘制每个联苯分子中间位和对位氯的数量(氯摩尔数/多氯联苯摩尔数)与沉积物年龄的关系图来确定脱氯速率。回归分析表明间位和对位氯浓度与时间之间存在线性相关性。平均脱氯速率为0.094±0.063摩尔氯/摩尔多氯联苯/年。使用2001年岩芯测得的速率大约是使用2000年岩芯测得速率的两倍,很可能是因为2001年的岩芯仅在断面O、L和I采集,而这些断面在2000年测得的速率最高。脱氯速率的倒数表明,每去除一个间位和对位氯需要16.4±11.6年(每个氯去除所需时间范围为4.3至43.5年)。本研究确定的速率比使用哈德逊河和圣劳伦斯河沉积物的实验室微观研究报告的速率低1 - 2个数量级,这表明实验室实验报告的脱氯速率比原位发生的速率高得多。

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