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中国福建西北部土壤中二氯二苯三氯乙烷(DDT)及其代谢物的来源和转化途径。

Sources and transformation pathways for dichlorodiphenyltrichloroethane (DDT) and metabolites in soils from Northwest Fujian, China.

机构信息

State Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences, Wuhan 430074, China; School of Environmental Studies, China University of Geosciences, Wuhan 430074, China; Lancaster Environment Centre, Lancaster University, Lancaster LA1 4YQ, UK.

State Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences, Wuhan 430074, China.

出版信息

Environ Pollut. 2018 Apr;235:560-570. doi: 10.1016/j.envpol.2017.12.071. Epub 2018 Jan 9.

Abstract

Dicofol (2,2,2-trichloro-1,1-bis-(p-chlorophenyl)ethanol) found in the environment is not only a miticide originated from commercial use, but also a metabolite of dichlorodiphenyltrichloroethane (DDT), which is often overlooked. To verify the sources and transformation pathways of DDT and related metabolites in soils, we measured p,p'-(dicofol + DBP) (sum of p,p'-dicofol and 4,4'-dichlorobenzophenone), DDT and six metabolites in soils from Northwest Fujian, China. The ratios of 1,1,1-trichloro-2-(o-chlorophenyl)-2-(p-chlorophenyl)ethane (o,p'-DDT)/1,1,1-trichloro-2,2-bis-(p-chlorophenyl)ethane (p,p'-DDT) and the mass balance demonstrated that p,p'-(dicofol + DBP) predominantly originated from p,p'-DDT transformation rather than from actual dicofol application. p,p'-(dicofol + DBP) accounted for 45.0% as the primary metabolites of DDT in this study, more than 1,1-dichloro-2,2-bis-(p-chlorophenyl)ethylene (p,p'-DDE) and 1,1-dichloro-2,2-bis-(p-chlorophenyl)ethane (p,p'-DDD), which might lead to large overestimations of the fresh DDT input by using the traditional ratio of (∑DDD + ∑DDE)/∑DDT (with all o,p'- and p,p'- isomers included). In paddy fields where the conditions alternate between aerobic (dry period) and anaerobic (wet period), both p,p'-DDD and p,p'-DDE were likely to degrade to 1-chloro-2,2-bis-(p-chlorophenyl)ethylene (p,p'-DDMU), which further transformed to 2,2-bis(p-chlorophenyl)ethylene (p,p'-DDNU). Degradation of p,p'-DDMU to p,p'-DDNU mainly occurred in waterlogged paddy soils. However, p,p'-DDNU might not transform to other higher-order metabolites in aerobic surface soils. Overall, our study confirmed p,p'-(dicofol + DBP) as metabolites of p,p'-DDT, suggested DDE and DDD were parallel precursors of DDMU, and further verified the transformation pathways of DDT in surface soils.

摘要

环境中二氯苯醚菊酯(2,2,2-三氯-1,1-双-(对氯苯基)乙醇)不仅是一种源于商业用途的杀螨剂,还是常常被忽视的滴滴涕(DDT)的一种代谢物。为了验证土壤中滴滴涕和相关代谢物的来源和转化途径,我们测量了来自中国福建西北部土壤中的 p,p'-(二氯苯醚菊酯+DBP)(p,p' -二氯苯醚菊酯和 4,4'-二氯二苯甲酮的总和)、滴滴涕和六种代谢物。1,1,1-三氯-2-(邻氯苯基)-2-(对氯苯基)乙烷(o,p'-DDT)/1,1,1-三氯-2,2-双-(对氯苯基)乙烷(p,p'-DDT)的比值和质量平衡表明,p,p'-(二氯苯醚菊酯+DBP)主要来源于 p,p'-DDT 的转化,而不是实际的二氯苯醚菊酯的使用。在本研究中,p,p'-(二氯苯醚菊酯+DBP)作为滴滴涕的主要初级代谢物,占比 45.0%,超过了 1,1-二氯-2,2-双-(对氯苯基)乙烯(p,p'-DDE)和 1,1-二氯-2,2-双-(对氯苯基)乙烷(p,p'-DDD),这可能会导致传统的(∑DDD+∑DDE)/∑DDT 比值(包含所有 o,p'-和 p,p'-异构体)对新鲜滴滴涕输入的高估。在水稻田中,条件在有氧(干燥期)和无氧(湿期)之间交替,p,p'-DDD 和 p,p'-DDE 都有可能降解为 1-氯-2,2-双-(对氯苯基)乙烯(p,p'-DDMU),然后进一步转化为 2,2-双(对氯苯基)乙烯(p,p'-DDNU)。在水淹稻田土壤中,p,p'-DDMU 向 p,p'-DDNU 的降解主要发生。然而,p,p'-DDNU 可能不会在有氧表土中转化为其他更高阶的代谢物。总的来说,我们的研究证实了 p,p'-(二氯苯醚菊酯+DBP)是 p,p'-DDT 的代谢物,表明 DDE 和 DDD 是 DDMU 的平行前体,并进一步验证了滴滴涕在表土中的转化途径。

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