Jörundsdóttir Hrönn, Norström Karin, Olsson Mats, Pham-Tuan Hai, Hühnerfuss Heinrich, Bignert Anders, Bergman Ake
Department of Environmental Chemistry, Stockholm University, SE-106 91 Stockholm, Sweden.
Environ Pollut. 2006 May;141(2):226-37. doi: 10.1016/j.envpol.2005.08.054. Epub 2005 Oct 12.
The dynamics of organohalogen contaminants and their metabolites are best studied over time by analysis of biota at high trophic levels. In this study, time trends, 1971-2001, of bis(4-chlorophenyl) sulfone (BCPS) and of methylsulfonyl-substituted metabolites of PCBs and 4,4'-DDE, were investigated in eggs of guillemot (Uria aalge) hatching in the Baltic Proper. Temporal trends of PCBs, trans-nonachlor, beta-HCH, 4,4'-DDT, and 4,4'-DDE were also assessed. Tris(4-chlorophenyl) methane (TCPMe), a 4,4'-DDT by-product, was detected in the eggs. The concentration of BCPS ranged between 2.6-0.76 microg/g on a lipid weight basis over the three decades and showed a significant 1.6% annual decrease. Three metabolites of PCBs, i.e. 3'-MeSO2-CB101, 4'-MeSO2-CB101 and 4-MeSO2-CB149, were quantified in all samples over time and showed an annual decrease of approximately 3% compared to MeSO2-DDE with a decrease of 8.9%. The methylsulfonyl-PCB and -DDE metabolites are eliminated more slowly than the persistent PCB congeners and 4,4'-DDE. Trans-nonachlor decreases by 16% compared to 19% and 9% for 4,4'-DDT and beta-HCH, respectively. The concentration of TCPMe in guillemot decreased by 8.2% per year. A linear relationship was found between TCPMe and 4,4'-DDE concentrations which supports the theory that TCPMe has an origin as a contaminant in commercial 4,4'-DDT products. The very slow decrease in BCPS concentrations is notable and remains to be explained. BCPS is still present at rather high concentrations in the guillemot eggs. The enantiomeric fraction varied between 0.27 and 0.67 which indicates less of a specific retention of the chiral MeSO2-PCBs in guillemot eggs than in grey seal tissues, for example. Independent of meta- or para-substitution of the sulfone group, the most accumulative atropisomer of each of four MeSO2-PCB pairs has been assigned an absolute R structure.
通过分析高营养级生物群随时间的变化，能最好地研究有机卤化物污染物及其代谢物的动态变化。在本研究中，调查了1971 - 2001年波罗的海中部海鸠（乌燕鸥）孵化卵中双（4 - 氯苯基）砜（BCPS）以及多氯联苯和4,4'-滴滴伊的甲基磺酰基取代代谢物的时间趋势。还评估了多氯联苯、反式九氯、β - 六氯环己烷、4,4'-滴滴涕和4,4'-滴滴伊的时间趋势。在卵中检测到了4,4'-滴滴涕的副产物三（4 - 氯苯基）甲烷（TCPMe）。在三十年期间，以脂质重量计，BCPS的浓度在2.6 - 0.76微克/克之间，且每年显著下降1.6%。随着时间推移，在所有样本中对三种多氯联苯代谢物，即3'-MeSO2 - CB101、4'-MeSO2 - CB101和4 - MeSO2 - CB149进行了定量，与下降8.9%的MeSO2 - DDE相比，它们每年下降约3%。甲基磺酰基多氯联苯和多氯联苯醚代谢物的消除速度比持久性多氯联苯同系物和4,4'-滴滴伊慢。与4,4'-滴滴涕下降19%和β - 六氯环己烷下降9%相比，反式九氯下降了16%。海鸠卵中TCPMe的浓度每年下降8.2%。发现TCPMe和4,4'-滴滴伊浓度之间存在线性关系，这支持了TCPMe源自商业4,4'-滴滴涕产品中污染物的理论。BCPS浓度下降非常缓慢，这一点值得注意且有待解释。BCPS在海鸠卵中仍以相当高的浓度存在。对映体分数在0.27至0.67之间变化，这表明例如在海鸠卵中手性MeSO2 - 多氯联苯的特异性保留比在灰海豹组织中少。无论砜基团的间位或对位取代情况如何，四个MeSO2 - 多氯联苯对中每一个的最具累积性的阻转异构体都被指定为绝对R结构。
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