紫色土干湿交替条件下邻苯二甲酸二甲酯迁移释放研究
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摘要
以三峡库区消落带典型土壤(紫色土)为对象,探讨消落带干湿交替过程中邻苯二甲酸二甲酯(DMP)在上覆水-间隙水-土壤之间的迁移释放特征。结果表明:土壤中DMP含量在两次淹水初期(0～2 d)明显下降,从第3天有反弹增高的趋势;间隙水、上覆水中DMP浓度总体呈现出微弱的增加、降低、再增加、再降低的振荡变化;两次落干初期(0～1 d),土壤中DMP均有不同程度的上升,在2～4 d有不同程度的下降,8～20 d时基本稳定在同一水平。土壤中初始DMP含量10～100mg·kg-1淹水后在三相间的迁移释放趋势相似,然而当土壤初始DMP含量增加至200 mg·kg-1后,上覆水DMP含量出现了与其他三组不同的变化趋势,三相间DMP的分配波动更大。准二级动力学方程可以很好地描述间隙水和上覆水中DMP向土壤中迁移的过程,相关性分析表明,间隙水和上覆水DMP浓度存在显著正相关的关系(P<0.05),而土壤与间隙水中DMP浓度呈现较弱的负相关。
【Objective】This paper is to characterize dimethyl phthalate(DMP) migration and release between overlying water, pore water and soil in the water level fluctuating zone of the Three-Gorges Reservoir during the wetting-drying alternation period.【Method】For the study a flooding experimental device was designed to carry out cyclical wet-dry alternation test using the "flooding-drying" model. 【Result】DMP content was found decreasing significantly in the soil during the first days(0～2 d) of the two flooding periods, but increasing from the third day on, and fluctuating slightly in the pore water and overlying water;it displayed a rising trend to a varying extent in the soil on the first days(0～1 d) of the two drying periods, and a declining one varying in degree on the following two days(2～4 d), and then leveled off during the late period(8～20 d). Soils with initial DMP content varying in the range of 10～100 mg·kg-1, when flooded, showed a similar trend in DMP migration and release between the three phases. However, DMP content in the overlying water showed a different trend from the other three groups, and the DMP distribution fluctuated greatly in the three phases,when soil initial DMP content was 200 mg·kg-1.【Conclusion】The quasi-second-order kinetic equation can be used to well describe migration of DMP in pore water and overlying water into the soil. Correlation analysis shows a significant positive correlation(P<0.05) exists between pore water and overlying water in DMP concentration, but a mildly negative one between soil and pore water.
【Objective】This paper is to characterize dimethyl phthalate(DMP) migration and release between overlying water, pore water and soil in the water level fluctuating zone of the Three-Gorges Reservoir during the wetting-drying alternation period.【Method】For the study a flooding experimental device was designed to carry out cyclical wet-dry alternation test using the "flooding-drying" model. 【Result】DMP content was found decreasing significantly in the soil during the first days(0～2 d) of the two flooding periods, but increasing from the third day on, and fluctuating slightly in the pore water and overlying water;it displayed a rising trend to a varying extent in the soil on the first days(0～1 d) of the two drying periods, and a declining one varying in degree on the following two days(2～4 d), and then leveled off during the late period(8～20 d). Soils with initial DMP content varying in the range of 10～100 mg·kg-1, when flooded, showed a similar trend in DMP migration and release between the three phases. However, DMP content in the overlying water showed a different trend from the other three groups, and the DMP distribution fluctuated greatly in the three phases,when soil initial DMP content was 200 mg·kg-1.【Conclusion】The quasi-second-order kinetic equation can be used to well describe migration of DMP in pore water and overlying water into the soil. Correlation analysis shows a significant positive correlation(P<0.05) exists between pore water and overlying water in DMP concentration, but a mildly negative one between soil and pore water.
引文
[1]刘文军，高健鹏，王冠颖，等. DEHP对土壤蚯蚓氧化胁迫及DNA损伤的研究.土壤学报，2017,54(5):1170—1180Liu W J,Gao J P,Wang G Y,et al. Oxidating stress and DNA damage of DEHP to soil earthworm(In Chinese). Acta Pedologica Sinica,2017,54(5):1170—1180
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[10]王勇，吴金清，黄宏文，等．三峡库区消涨带植物群落的数量分析.武汉植物学研究，2004,22(4):307—314Wang Y,Wu J Q,Huang H W,et al. Quantitative analysis of plant communities in water-level-?uctuation zone within Three Gorges Reservoir Area of Changjiang River(In Chinese).Journal of Wuhan Botanical Research,2004,22(4):307—314
[11]陈济安，邱志群，舒为群，等.我国水环境中邻苯二甲酸酯污染现状及其生物降解研究进展.癌变畸变突变，2007,19(3):212—214Chen J A,Qiu Z Q,Shu W Q,et al. Pollution of PAEs in water and the biodegradations studies in China(In Chinese). Carcinogenesis Teratogenesis&Mutagenesis,2007,19(3):212—214
[12]王凡，沙玉娟，夏星辉，等.长江武汉段水体邻苯二甲酸酯分布特征研究.环境科学，2008,29(5):1163—1169Wang F,Sha Y J,Xia X H,et al. Distribution characteristics of phthalic acid esters in the Wuhan section of Yangtze River(In Chinese). Environmental Science,2008,29(5):1163—1169
[13]林莉，董磊，李青云，等.三峡库区水体和底泥中多环芳烃和邻苯二甲酸酯类分布和来源.湖泊科学，2018,30(3):660—667Lin L,Dong L,Li Q Y,et al. Distribution and sources of polycyclic aromatic hydrocarbons and phthalic acid esters in water and surface sediment from the Three Gorges Reservoir(In Chinese). Journal of Lake Sciences,2018,30(3):660—667
[14]杨婷，何明靖，杨志豪，等.邻苯二甲酸酯在三峡库区消落带非淹水期土壤中污染特征及健康风险.环境科学，2017,38(10):4187—4193Yang T,He M J,Yang Z H,et al. Occurrence,distribution and health risk of the phthalate esters in riparian soil in the?uctuating zone of the Three Gorges Reservoir(In Chinese). Environmental Science,2017,38(10):4187—4193
[15]王莲阁，高岩红，丁长欢，等.三峡库区典型消落带土壤有机碳分布特征.西南大学学报（自然科学版），2015,37(3):120—124Wang L G,Gao Y H,Ding C H,et al. Distribution characteristics of soil organic carbon in a typical water-level-fluctuation zone of the Three Gorges Reservoir area(In Chinese). Journal of Southwest University(Natural Science Edition),2015,37(3):120—124
[16]胥焘，王飞，郭强，等.三峡库区香溪河消落带及库岸土壤重金属迁移特征及来源分析.环境科学，2014,35(4):1502—1508Xu T,Wang F,Guo Q,et al. Transfer characteristic and source identi?cation of soil heavy metals from water-level-?uctuating zone along Xiangxi river,Three-Gorges Reservoir area(In Chinese). Environmental Science,2014,35(4):1502—1508
[17]杨茜，石艳，江韬，等.有机酸对三峡库区消落带土壤无机磷形态转化和有效性的影响.水土保持学报，2015, 29(4):272—277Yang X,Shi Y,Jiang T,et al. Effect of organic acids on form transformation and availability of soil inorganic phosphorous in the water-fluctuation zone of Three Gorges Reservoir area(In Chinese). Journal of Soil and Water Conservation,2015,29(4):272—277
[18]杜娴.重庆主城两江水体与沉积物中邻苯二甲酸酯和多环芳烃污染水平及特征.重庆：重庆大学，2012Du X. Levels and characteristics of phthalate esters and polycyclic aromatic hydrocarbons in the Yangtze River and Jialing River from Chongqing’s urban areas(In Chinese). Chongqing:Chongqing Univerity,2012
[19]杨志丹.三峡库区消落带邻苯二甲酸二丁酯迁移释放的静态模拟.重庆：西南大学，2014Yang Z D. The static simulation of dibutyl-phthalate migration and release in the?uctuating zone of Three Gorges Reservoir(In Chinese). Chongqing:Southwest University,2014
[20]曹琳，吉芳英，林茂，等.三峡库区干湿交替消落区土壤磷形态.长江流域资源与环境，2011,20(1):101—106Cao L,Ji F Y,Lin M,et al. Soil phosphorous from analysis in?uctuating(dry-wet cycling)zone of Three Gorges Reservoir(In Chinese). Resources and Environment in the Yangtze Basin,2011,20(1):101—106
[21]张金洋.三峡水库消落区土壤汞释放特征研究.重庆：西南农业大学，2005Zhang J Y. Study on release characteristic of mercury from soil in water level fluctuation zone of Three Gorges Reservoir(In Chinese). Chongqing:Southwest Agriculture University,2005
[22] U. S. Environmental Protection Agency. Method 3510C:Separatory funnel liquid-liquid extraction. 1996. https：//www.epa. gov/sites/production/?les/2015-12/documents/3510c. pdf
[23]马燕玲，陈令新，丁养军，等.超声辅助分散液液微萃取-高效液相色谱测定水样中的4种邻苯二甲酸酯类增塑剂.色谱，2013,31(2):155—161Ma Y L,Chen L X,Ding Y J,et al. Simultaneous determination of four phthalate esters in water samples using ultrasound-assisted dispersive liquid-liquid microextraction coupled with high performance liquid chromatography(In Chinese). Chinese Journal of Chromatography,2013,31(2):155—161
[24]王法，王强，木志坚，等.三峡库区消落带土壤邻苯二甲酸二丁酯静态释放特征.环境科学，2015,36(7):2453—2458Wang F,Wang Q,Mu Z J,et al. Static migration and release of dibutyl-phthalate in the?uctuating zone of Three Gorges Reservoir(In Chinese). Environmental Science,2015,36(7):2453—2458
[25]丁辉，王胜强，孙津生，等.海河干流底泥中六氯苯残留及其释放规律.环境科学，2006,27(3):533—537Ding H,Wang S Q,Sun J S,et al. HCB residue and desorption kinetics of HCB in sediments from Haihe River main branch(In Chinese). Environmental Science,2006,27(3):533—537
[26]李晓娜，宋洋，贾明云，等.生物质炭对有机污染物的吸附及机理研究进展.土壤学报，2017,54(6):1313—1325Li X N,Song Y,Jia M Y,et al. A Review of researches on biochar adsorbing organic contaminants and its mechanism(In Chinese). Acta Pedologica Sinica,2017,54(6):1313—1325
[27]宋娇艳，木志坚，王强，等.环境条件对三峡库区消落带土壤中邻苯二甲酸二丁酯向上覆水静态迁移释放的影响.环境科学，2015,36(1):143—150Song J Y,Mu Z J,Wang Q,et al. Effect of external condition on the static migration and release of dibutyl-phthalate in the soil of the?uctuating zone of the Three Gorges Reservoir to the overlying water(In Chinese). Environmental Science,2015,36(1):143—150
[2] Schettler T. Human exposure to phthalates via consumer products.International Journal of Andrology,2006,29:134—139
[3] Gomez-Hens A,Aguilar-Caballos M. Social and economic interest in the control of phthalic acid esters. Trends in Analytical Chemistry,2003,22(11):847—857
[4] Petrovic M,Eljarrat E,Alda M J,et al. Endocrine disrupting compounds and other emerging contaminants in the environment:A survey on new monitoring strategies and occurrence data. Analytical and Bioanalytical Chemistry,2004,378:549—562
[5] Han D,Li J,Cao H,et al. Theoretical investigation on the mechanisms and kinetics of OH-initiated photooxidation of dimethyl phthalate(DMP)in atmosphere. Chemosphere,2014,95:50—57
[6] Ventrice P,Ventrice D,Russo E,et al. Phthalates:European regulation,chemistry,pharmacokinetic and related toxicity. Environmental Toxicology and Pharmacology,2013,36:88—96
[7] Xu B,Gao N Y,Cheng H,et al. Oxidative degradation of dimethyl phthalate(DMP)by UV/H2O2 process. Journal of Hazardous Materials,2008,162:954—959
[8] Bauer M J,Herrmann R. Estimation of the environmental contamination by phthalic acid esters leaching from household wastes. Science of the Total Environment,1997,208(1/2):49—57
[9] Wang J,Luo Y,Teng Y,et al. Soil contamination by phthalate esters in Chinese intensive vegetable production systems with different modes of use of plastic?lm. Environment Pollution,2013,180:265—273
[10]王勇，吴金清，黄宏文，等．三峡库区消涨带植物群落的数量分析.武汉植物学研究，2004,22(4):307—314Wang Y,Wu J Q,Huang H W,et al. Quantitative analysis of plant communities in water-level-?uctuation zone within Three Gorges Reservoir Area of Changjiang River(In Chinese).Journal of Wuhan Botanical Research,2004,22(4):307—314
[11]陈济安，邱志群，舒为群，等.我国水环境中邻苯二甲酸酯污染现状及其生物降解研究进展.癌变畸变突变，2007,19(3):212—214Chen J A,Qiu Z Q,Shu W Q,et al. Pollution of PAEs in water and the biodegradations studies in China(In Chinese). Carcinogenesis Teratogenesis&Mutagenesis,2007,19(3):212—214
[12]王凡，沙玉娟，夏星辉，等.长江武汉段水体邻苯二甲酸酯分布特征研究.环境科学，2008,29(5):1163—1169Wang F,Sha Y J,Xia X H,et al. Distribution characteristics of phthalic acid esters in the Wuhan section of Yangtze River(In Chinese). Environmental Science,2008,29(5):1163—1169
[13]林莉，董磊，李青云，等.三峡库区水体和底泥中多环芳烃和邻苯二甲酸酯类分布和来源.湖泊科学，2018,30(3):660—667Lin L,Dong L,Li Q Y,et al. Distribution and sources of polycyclic aromatic hydrocarbons and phthalic acid esters in water and surface sediment from the Three Gorges Reservoir(In Chinese). Journal of Lake Sciences,2018,30(3):660—667
[14]杨婷，何明靖，杨志豪，等.邻苯二甲酸酯在三峡库区消落带非淹水期土壤中污染特征及健康风险.环境科学，2017,38(10):4187—4193Yang T,He M J,Yang Z H,et al. Occurrence,distribution and health risk of the phthalate esters in riparian soil in the?uctuating zone of the Three Gorges Reservoir(In Chinese). Environmental Science,2017,38(10):4187—4193
[15]王莲阁，高岩红，丁长欢，等.三峡库区典型消落带土壤有机碳分布特征.西南大学学报（自然科学版），2015,37(3):120—124Wang L G,Gao Y H,Ding C H,et al. Distribution characteristics of soil organic carbon in a typical water-level-fluctuation zone of the Three Gorges Reservoir area(In Chinese). Journal of Southwest University(Natural Science Edition),2015,37(3):120—124
[16]胥焘，王飞，郭强，等.三峡库区香溪河消落带及库岸土壤重金属迁移特征及来源分析.环境科学，2014,35(4):1502—1508Xu T,Wang F,Guo Q,et al. Transfer characteristic and source identi?cation of soil heavy metals from water-level-?uctuating zone along Xiangxi river,Three-Gorges Reservoir area(In Chinese). Environmental Science,2014,35(4):1502—1508
[17]杨茜，石艳，江韬，等.有机酸对三峡库区消落带土壤无机磷形态转化和有效性的影响.水土保持学报，2015, 29(4):272—277Yang X,Shi Y,Jiang T,et al. Effect of organic acids on form transformation and availability of soil inorganic phosphorous in the water-fluctuation zone of Three Gorges Reservoir area(In Chinese). Journal of Soil and Water Conservation,2015,29(4):272—277
[18]杜娴.重庆主城两江水体与沉积物中邻苯二甲酸酯和多环芳烃污染水平及特征.重庆：重庆大学，2012Du X. Levels and characteristics of phthalate esters and polycyclic aromatic hydrocarbons in the Yangtze River and Jialing River from Chongqing’s urban areas(In Chinese). Chongqing:Chongqing Univerity,2012
[19]杨志丹.三峡库区消落带邻苯二甲酸二丁酯迁移释放的静态模拟.重庆：西南大学，2014Yang Z D. The static simulation of dibutyl-phthalate migration and release in the?uctuating zone of Three Gorges Reservoir(In Chinese). Chongqing:Southwest University,2014
[20]曹琳，吉芳英，林茂，等.三峡库区干湿交替消落区土壤磷形态.长江流域资源与环境，2011,20(1):101—106Cao L,Ji F Y,Lin M,et al. Soil phosphorous from analysis in?uctuating(dry-wet cycling)zone of Three Gorges Reservoir(In Chinese). Resources and Environment in the Yangtze Basin,2011,20(1):101—106
[21]张金洋.三峡水库消落区土壤汞释放特征研究.重庆：西南农业大学，2005Zhang J Y. Study on release characteristic of mercury from soil in water level fluctuation zone of Three Gorges Reservoir(In Chinese). Chongqing:Southwest Agriculture University,2005
[22] U. S. Environmental Protection Agency. Method 3510C:Separatory funnel liquid-liquid extraction. 1996. https：//www.epa. gov/sites/production/?les/2015-12/documents/3510c. pdf
[23]马燕玲，陈令新，丁养军，等.超声辅助分散液液微萃取-高效液相色谱测定水样中的4种邻苯二甲酸酯类增塑剂.色谱，2013,31(2):155—161Ma Y L,Chen L X,Ding Y J,et al. Simultaneous determination of four phthalate esters in water samples using ultrasound-assisted dispersive liquid-liquid microextraction coupled with high performance liquid chromatography(In Chinese). Chinese Journal of Chromatography,2013,31(2):155—161
[24]王法，王强，木志坚，等.三峡库区消落带土壤邻苯二甲酸二丁酯静态释放特征.环境科学，2015,36(7):2453—2458Wang F,Wang Q,Mu Z J,et al. Static migration and release of dibutyl-phthalate in the?uctuating zone of Three Gorges Reservoir(In Chinese). Environmental Science,2015,36(7):2453—2458
[25]丁辉，王胜强，孙津生，等.海河干流底泥中六氯苯残留及其释放规律.环境科学，2006,27(3):533—537Ding H,Wang S Q,Sun J S,et al. HCB residue and desorption kinetics of HCB in sediments from Haihe River main branch(In Chinese). Environmental Science,2006,27(3):533—537
[26]李晓娜，宋洋，贾明云，等.生物质炭对有机污染物的吸附及机理研究进展.土壤学报，2017,54(6):1313—1325Li X N,Song Y,Jia M Y,et al. A Review of researches on biochar adsorbing organic contaminants and its mechanism(In Chinese). Acta Pedologica Sinica,2017,54(6):1313—1325
[27]宋娇艳，木志坚，王强，等.环境条件对三峡库区消落带土壤中邻苯二甲酸二丁酯向上覆水静态迁移释放的影响.环境科学，2015,36(1):143—150Song J Y,Mu Z J,Wang Q,et al. Effect of external condition on the static migration and release of dibutyl-phthalate in the soil of the?uctuating zone of the Three Gorges Reservoir to the overlying water(In Chinese). Environmental Science,2015,36(1):143—150
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