近百年来大辽河口潮间带中滴滴涕(DDTs)的沉积记录及其对人类活动的响应
Sediment records of DDTs in intertidal sediment core of Daliao River Estuary and their responses to anthropogenic activities in the past century
-
摘要: 滴滴涕(DDTs)在中国农业生产中的使用已被禁止30多年,但仍在多种环境介质中有检出.潮间带作为陆地与海洋交汇区,是污染物在环境中重要的汇.为全面了解近百年来大辽河口潮间带中DDTs的沉积特征,本研究通过在大辽河口潮间带采集柱状沉积物样品,结合定年结果,揭示了近百年来大辽河口潮间带柱状沉积物中DDTs的污染特征,并对其潜在风险、源趋和影响因素进行了分析.结果显示,大辽河口潮间带柱状沉积物中DDTs浓度范围为0.313—4.116 ng·g-1(中值:2.061 ng·g-1),以p,p'-DDTs为主要污染物.1988—1996年为沉积物中DDTs污染高峰期(3.436—4.116 ng·g-1),与1971—1981年农药生产高峰期相对应,且存在约15年的延迟.2000年以后,辽宁省可能存在工业DDT的使用,且与疾病防控有关.经风险评估发现,DDT和DDE在0—110 cm范围内均极少(<25%)对底栖生物产生负效应,而DDD和总DDTs在0—44 cm范围内偶尔(25%—50%)对底栖生物产生负效应.DDTs的特征比值分析表明,大辽河口潮间带沉积柱中DDTs主要来源于工业DDT的历史污染而非三氯杀螨醇的使用.DDT降解产物在深层(62—110 cm)以DDE为主,而在浅层(0—62 cm)以DDD为主.1971年后人为活动导致TOC含量的增加是促使大辽河口潮间带沉积物由好氧环境转变为厌氧环境的重要因素.此外,大辽河口潮间带沉积物中DDTs浓度与沉积物性质(总氮(TN)、总磷(TP)和总有机碳(TOC))具有极显著相关性(P<0.01),且与辽宁省GDP、城市化率和农业总产值等人为活动具有极显著正相关性(P<0.01).综上,由潮间带沉积柱中DDTs的浓度和组成反映出人类活动直接或间接影响了潮间带中污染物的存在和归趋.Abstract: Dichlorodiphenyltrichloroethanes (DDTs) are still detected in various environmental matrices, although their usage in agriculture has been banned for about 30 years in China. Intertidal zone, as the intersection area of land and sea, is the final sink for contaminants. To comprehensively understand the deposition features of DDTs in intertidal sediment of Daliao River Estuary, a sediment core was sampled in this study. Combined with the dating data, the distribution, potential risk, source and fate of DDTs were investigated. The results showed that DDTs concentrations ranged from 0.313 ng·g-1 to 4.116 ng·g-1(median:2.061 ng·g-1), with p,p'-DDTs being the major components. Interestingly, the peak of DDTs concentrations (3.436-4.116 ng·g-1) during 1988-1996 corresponded well with the peak of pesticide production during 1971-1981, and a 15-year-round time lag was observed between these two peaks. Possible usage of technical DDT was implied after year 2000 for the control and prevention of disease in Liaoning Province. The risk assessment of DDTs revealed that concentrations of DDT and DDE in sediment core rarely (<25%) showed negative effect, while concentrations of DDD and total DDTs in the depth of 0-44 cm occasionally (25%-50%) showed negative effect. The specific ratios of DDTs demonstrated that DDTs in the intertidal sediments were mainly from historical use of technical DDT rather than the use of dicofol. DDE and DDD were the main degradation products of DDT in the deeper layer (62-110 cm) and shallower layer (0-61 cm), respectively. Further analysis revealed that the increased TOC content caused by human activities after year 1971 was the main reason that led the sediment environment changing from aerobic environment to anaerobic environment. What's more, DDTs concentrations in sediment core had strong positive correlations with sediment properties (TN, TP and TOC) (P<0.01), and also had a significant positive correlation with anthropogenic activities (such as GDP, urbanization and total agricultural output value) (P<0.01). Therefore, the results of the concentrations and compositions of DDTs in intertidal sediment core could reflect the direct and indirect influence of human activities on the occurrence and fate of contaminants in intertidal sediment.
-
[1] MENG J, HONG S, WANG T, et al. Traditional and new POPs in environments along the Bohai and Yellow Seas:An overview of China and South Korea[J]. Chemosphere, 2017, 169:503-515. [2] YAN S, WANG D, TENG M, et al. Perinatal exposure to low-dose decabromodiphenyl ethane increased the risk of obesity in male mice offspring[J]. Environmental Pollution, 2018, 243:553-562. [3] FANG Y, NIE Z, DIE Q, et al. Organochlorine pesticides in soil, air, and vegetation at and around a contaminated site in southwestern China:Concentration, transmission, and risk evaluation[J]. Chemosphere, 2017, 178:340-349. [4] LIU W X, WANG Y, HE W, et al. Aquatic biota as potential biological indicators of the contamination, bioaccumulation and health risks caused by organochlorine pesticides in a large, shallow Chinese lake (Lake Chaohu)[J]. Ecological Indicators, 2016, 60:335-345. [5] LIN T, HU Z, ZHANG G, et al. Levels and mass burden of DDTs in sediments from fishing harbors:The importance of DDT-containing antifouling paint to the coastal environment of China[J]. Environmental Science & Technology, 2009, 43(21):8033-8038. [6] LIU L Y, MA W L, JIA H L, et al. Research on persistent organic pollutants in China on a national scale:10 years after the enforcement of the Stockholm Convention[J]. Environmental Pollution, 2016, 217:70-81. [7] FUJII Y, HARAGUCHI K, HARADA K H, et al. Detection of dicofol and related pesticides in human breast milk from China, Korea and Japan[J]. Chemosphere, 2011, 82(1):25-31. [8] 叶晟, 孔飞, 李宏俊, 等. 辽河口邻近海域小型底栖生物的空间分布及季节变化[J]. 海洋学报, 2017, 39(10):78-89. YE C, KONG F, LI H J, et al. Spatial distribution and season variation of meiobenthos community in the Liaohe Estuary[J]. Haiyang Xuebao, 2017, 39(10):78-89(in Chinese).
[9] GAO X Y, JIAO J, DOU X P, et al. Study on sedimentation for waterway regulation of the Daliao River Estuary[C]. in Asian and Pacific Coasts 2017:Proceedings of the 9th International Conference on APAC 2017. Singapore:World Scientific Publishing Co Pte Ltd., 2018. [10] LIU J, SUN Q, MO C, et al. The pollution status and characteristics of Daliaohe Estuary and its adjacent sea area[J]. Fisheries Science, 2008, 27(6):286-289. [11] TAN L, HE M C, MEN B, et al. Distribution and sources of organochlorine pesticides in water and sediments from Daliao River estuary of Liaodong Bay, Bohai Sea (China)[J]. Estuarine Coastal and Shelf Science, 2009, 84(1):119-127. [12] DA C N, LIU G J, SUN R Y, et al. Sources and risk assessment of organochlorine pesticides in surface soils from the nature reserve of the Yellow River Delta, China[J]. Soil Science Society of America Journal, 2014, 78(3):779-786. [13] LIU M, CHENG S, OU D, et al. Organochlorine pesticides in surface sediments and suspended particulate matters from the Yangtze estuary, China[J]. Environmental Pollution, 2008, 156(1):168-173. [14] WU Y, WANG X, YA M, et al. Distributions of organochlorine compounds in sediments from Jiulong River Estuary and adjacent Western Taiwan Strait:Implications of transport, sources and inventories[J]. Environmental Pollution, 2016, 219:519-527. [15] PENG L, DAI X, YU A. Assessment of the spatial and temporal distribution of legacy persistent organic pollutants and recommendations for sample collection from the surficial sediments of estuaries and seas in China[J]. Chemosphere, 2015, 119 Suppl:S138-144. [16] LEBEUF M, NUNES T. PCBs and OCPs in sediment cores from the Lower St. Lawrence Estuary, Canada:Evidence of fluvial inputs and time lag in delivery to coring sites[J]. Environmental Science & Technology, 2005, 39(6):1470-1478. [17] SHEN B B, WU J L, ZHAO Z H. A similar to 150-year record of human impact in the Lake Wuliangsu (China) watershed:Evidence from polycyclic aromatic hydrocarbon and organochlorine pesticide distributions in sediments[J]. Journal of Limnology, 2016, 76(1):129-136. [18] YUAN H, LIU E, ZHANG E, et al. Historical records and sources of polycyclic aromatic hydrocarbons (PAHs) and organochlorine pesticides (OCPs) in sediment from a representative plateau lake, China[J]. Chemosphere, 2017, 173:78-88. [19] YANG R Q, XIE T, YANG H D, et al. Historical trends of organochlorine pesticides (OCPs) recorded in sediments across the Tibetan Plateau[J]. Environmental Geochemistry and Health, 2018, 40(1):303-312. [20] WANG W, BAI J, ZHANG G, et al. Depth-distribution, possible sources, and toxic risk assessment of organochlorine pesticides (OCPs) in different river sediment cores affected by urbanization and reclamation in a Chinese delta[J]. Environmental Pollution, 2017, 230:1062-1072. [21] 滕聪, 雷露, 孙英伟, 等. 2008-2013年辽宁省疟疾流行病学分析[J]. 中国血吸虫病防治杂志, 2014, 26(2):200-202. TENG C, LEI L, SUN Y W, et al. Prevalence of malaria in Liaoning Province, 2008 to 2013[J]. Chinese Journal of Schistosomiasis Control, 2014, 26(2):200-202(in Chinese).
[22] 咸越, 刘春燕, 贺知菲, 等. 中国2009-2014年疟疾疫情流性特征分析[J]. 中国公共卫生, 2017, 33(4):517-519. XIAN Y, LIU C Y, HE Z F, et al. Epidemic characteristic of malaria in China:2009-2014[J]. Chinese Journal of Public Health, 2017, 33(4):517-519(in Chinese).
[23] 周军. 夏季猪场蚊虫的防控[J]. 当代畜牧, 2009(5):54-56. ZHOU J. Prevention and control of mosquitoes in pig farms in summer[J]. Contemporary Animal Husbandry, 2009 (5):54-56(in Chinese).
[24] CCME. Canadian sediment quality guidelines for the protection of aquatic life:DDT, DDE, and DDD[S]. Canadian Environmental Quality Guidelines, 1999. [25] YU H Y, ZHANG B Z, GIESY J P, et al. Persistent halogenated compounds in aquaculture environments of South China:Implications for global consumers' health risk via fish consumption[J]. Environment International, 2011, 37(7):1190-1195. [26] WU Y, WANG X, YA M, et al. Distributions of organochlorine compounds in sediments from Jiulong River Estuary and adjacent Western Taiwan Strait:Implications of transport, sources and inventories[J]. Environmental Pollution, 2016, 219:519-527. [27] QIU X, ZHU T. Using the o,p'-DDT/p,p'-DDT ratio to identify DDT sources in China[J]. Chemosphere, 2010, 81(8):1033-1038. [28] LIU L, BAI L, MAN C, et al. DDT vertical migration and formation of accumulation layer in pesticide-producing sites[J]. Environmental Science & Technology, 2015, 49(15):9084-9091. [29] LIU W, CHEN J, HU J, et al. Multi-residues of organic pollutants in surface sediments from littoral areas of the Yellow Sea, China[J]. Marine Pollutution Bulletin, 2008, 56(6):1091-1103. [30] ZHOU S, YANG H, ZHANG A, et al. Distribution of organochlorine pesticides in sediments from Yangtze River Estuary and the adjacent East China Sea:Implication of transport, sources and trends[J]. Chemosphere, 2014, 114:26-34. [31] LIU M, CHENG S, OU D, et al. Organochlorine pesticides in surface sediments and suspended particulate matters from the Yangtze estuary, China[J]. Environmental Pollution, 2008, 156(1):168-173. [32] 王雅苹. 青岛潮间带沉积物厌氧细菌的分离培养和多样性研究[D]. 青岛:中国海洋大学, 2014. WANG Y P. Study on isolation and diversity of culturable anaerobic bacteria in intertidal sediment of Qingdao[D]. Qingdao, Ocean University of China, 2014(in Chinese). [33] [34] 李学刚, 宋金明, 李宁, 等. 胶州湾沉积物中氮与磷的来源及其生物地球化学特征[J]. 海洋与湖沼, 2005, 36(6):562-571. LI X G, SONG J M, LI N, et al. Source and biogeochemical characteristics of nitrogen and phosphorus in Jiaozhou bay sediments[J]. Oceanologia et Limnologia Sinica, 2005, 36(6):562-571(in Chinese).
[35] RAVINDRA K, SOKHI R, VANGRIEKEN R. Atmospheric polycyclic aromatic hydrocarbons:Source attribution, emission factors and regulation[J]. Atmospheric Environment, 2008, 42(13):2895-2921.
计量
- 文章访问数: 1427
- HTML全文浏览数: 1427
- PDF下载数: 47
- 施引文献: 0