冻融条件下溶解性有机物在冰-水-沉积物体系中的迁移
作者:
作者单位:

重庆大学环境与生态学院

中图分类号:

X522

基金项目:

国家重点研发计划课题(2019YFD1100501)


Migration of dissolved organic matter in an ice-water-sediment system under freeze-thaw alternating conditions
Author:
Affiliation:

College of Environment and Ecology, Chongqing University

Fund Project:

National Key R&D Program of China

  • 摘要
  • | |
  • 访问统计
  • |
  • 参考文献 [28]
  • | | | |
  • 文章评论
    摘要:

    目的:目前关于地表水冰封的研究主要集中于冰封期重金属、营养盐在冰-水体系的分布特征,室内模拟实验则侧重于研究冻融过程中污染物在冰-水体系中的迁移规律及其影响因素。冻融条件下污染物在冰-水-沉积物体系中的迁移规律,尚未明了。因此本文以溶解性有机物(DOM)为研究对象,探究溶解性污染物在冰-水-沉积物体系中的分布变化规律。结合总氮(TN)、总磷(TP)等指标分析不同物质在冻融过程中的关联特征,以环境雌激素类非挥发性有机微污染物为特征污染物,剖析其在冰水相变过程中的浓度变化动态特征。 方法:设置室内控制实验,测定冻融过程中冰水两相的三维荧光光谱(EEMs)、比紫外吸光度(SUVA254)、总氮(TN)、总磷(TP)、溶解有机碳(DOC),并对三维荧光特征指数、SUVA254、TN、TP、DOC进行相关性分析。在排除沉积物影响的前提下,测定冻融过程中冰水两相双酚A(BPA)、雌二醇(E2)、炔雌醇(EE2)的浓度。 结果:1)冻结过程中水相的三维荧光光谱中类色氨酸峰、类酪氨酸峰、类腐殖酸峰的荧光强度增强,TN、TP浓度增加至原水样的1.47、1.13倍,说明在冻结过程中由于冷冻浓缩效应,类色氨酸、类酪氨酸、类腐殖酸三类溶解性有机物、TN、TP由冰相向水相迁移。在水体完全冻结时,冰相的类色氨酸峰、类酪氨酸峰、类腐殖酸峰荧光强度小于原水样,TN、TP浓度降低至原水样的0.76、0.87倍,说明三类溶解性有机物、TN、TP进一步向沉积物迁移,最后在溶解过程中,由沉积物向水体释放。但溶解过程中沉积物向水体释放的三类溶解性有机物、TP的量少于冻结过程中迁移的量,意味着部分污染物在此过程中富集在沉积物中。2)通过测定冻融条件下冰水两相中BPA、E2、EE2的浓度发现,在冻结过程中BPA、E2、EE2向水相中迁移,但迁移速率有所不同。3)相关性分析结果表明,在冻融过程中SUVA254和TP显著正相关,在冻融的影响下,芳香族物质与含P溶解性物质迁移趋势的关联较为紧密。 结论:在冻结过程中,污染物尤其是芳香类污染物向沉积物迁移并富集在沉积物中。冰体融化过程中,在温度、外界扰动的影响下污染物由沉积物向水体释放。因此在地表水冰层形成过程中,冰下水体中污染物浓度升高,同时水体中污染物向沉积物迁移,停留在沉积物中。春季冰层融化,停留在沉积物中的污染物向水体释放,导致春季地表水中污染物浓度升高,可能对水生生态系统健康构成潜在风险。

    Abstract:

    Objectives: At present, the research on the freezing of surface water mainly focuses on the distribution characteristics of heavy metals and nutrients in ice-water systems during the freezing period. The indoor simulation experiments focus on the migration and influencing factors of pollutants in ice-water systems during freeze-thaw process. However, the migration of pollutants in ice-water-sediment systems under freeze-thaw alternating conditions remain unclear. In the current study, the dissolved organic matter (DOM) was selected as the study object to explore the distribution and migration of dissolved pollutants in an ice-water-sediment system. Combined with total nitrogen (TN), total phosphorus (TP) and other indicators, the correlation characteristics of different substances in freeze-thaw process were analyzed. In addition, environmental estrogens were chosen as represented microorganic pollutants to illustrate the variation on concentrations between ice and water phase during the freeze-thaw alternating process. Methods: Indoor control experiments were set up to measure the three-dimensional fluorescence spectra (EEMs), specific ultraviolet absorbance (SUVA254), and concentrations of total nitrogen (TN), total phosphorus (TP) and dissolved organic carbon (DOC) in ice and water during freeze-thaw process, and the correlation analysis among three-dimensional fluorescence characteristic index, SUVA254, TN, TP and DOC was performed. Simultaneously, the concentrations of bisphenol A (BPA), estradiol (E2) and ethinyl estradiol (EE2) in an ice-water system during freeze-thaw process were measured. Results: 1) The fluorescence intensity peaks of tryptophan-like, tyrosine-like and humic acid-like compounds in the three-dimensional fluorescence spectrum of aqueous phase increased during freezing process, and the concentrations of TN and TP increased to 1.47 and 1.13 times of the raw water sample. The results indicated that tryptophan-like, tyrosine-like and humic acid-like dissolved organic matters, TN and TP migrated from ice phase to aqueous phase due to the freeze concentration effect. When the water was completely frozen, the fluorescence intensity peaks of tryptophan-like, tyrosine-like and humic acid-like compounds at ice phase was lower than that of the raw water sample, and the concentrations of TN and TP were reduced to 0.76 and 0.87 times as compared to the raw water sample, which indicates that those three kinds of dissolved organic matters, TN and TP migrated to the sediment, and then released from the sediment to the water body during dissolution process. However, the amount of those three kinds of dissolved organic matters and TP released from sediment to water in the process of dissolution was less than that transferred in the process of freezing, which means that some pollutants were enriched in sediment in this process. 2) By measuring the concentrations of BPA, E2 and EE2 in the ice-water phase under freeze-thaw alternating conditions, it was found that BPA, E2 and EE2 migrated to the water phase during freezing, but the migration rates were different. 3) The results of correlation analysis showed that SUVA254 was positively correlated with TP during freeze-thaw process. Under the influence of freezing and thawing, the migration trend of aromatic substances and phosphorus-containing dissolved substances is closely related. Conclusions: During the freezing process, pollutants, especially aromatic pollutants, were migrated to and accumulated in sediments. In the process of ice melting, pollutants are released from sediments to water under the influence of temperature and external disturbance. Therefore, during the formation of the surface water ice layer, the concentration of pollutants in the water under the ice increases, while pollutants migrated to the sediment and stay in the sediment. When the ice melts in spring, pollutants staying in sediments will release into water, which lead to the increase of pollutant concentration in surface water in spring and may pose potential risks to aquatic ecosystem health.

    参考文献
    [1] 高宁. 水体结冰和融冰过程中典型污染物的迁移规律研究[D]. 山东烟台: 烟台大学, 2018.
    [2] 杜丹丹,李畅游,史小红,等. 乌梁素海水体营养状态季节性变化特征研究[J]. 干旱区资源与环境, 2019, 33(12): 186-192.
    [3] He S, Dong D, Sun C, et al. Contaminants of emerging concern in a freeze-thaw river during the spring flood[J]. Science of the Total Environment, 2019, 670: 576-584.
    [4] Liu S, Wang Z, Lu K, et al. Melting scenario affects the dynamics of polycyclic aromatic hydrocarbons released from snowpack[J]. Environmental Research Letters, 2020, 15(6).
    [5] Chen Z L, Zhu Z H, Song J Y, et al. Linking biological toxicity and the spectral characteristics of contamination in seriously polluted urban rivers[J]. Environmental Sciences Europe, 2019, 31(1).
    [6] Li Y, Yang L, Zhen H, et al. Determination of estrogens and estrogen mimics by solid-phase extraction with liquid chromatography-tandem mass spectrometry[J]. Journal of Chromatography B, 2021, 1168.
    [7] De Liz M V, Do Amaral B, Stets S, et al. Sensitive Estrogens Determination in Wastewater Samples by HPLC and Fluorescence Detection[J]. JOURNAL OF THE BRAZILIAN CHEMICAL SOCIETY, 2017, 28(8): 1453-1460.
    [8] Yoon Y, Westerhoff P, Snyder S A, et al. HPLC-fluorescence detection and adsorption of bisphenol A, 17β-estradiol, and 17α-ethynyl estradiol on powdered activated carbon[J]. Water Research, 2003, 37(14): 3530-3537.
    [9] 张紫薇,周石磊,张甜娜,等. 岗南水库沉积物溶解性有机物光谱时空分布特征及环境意义[J]. 环境科学学报, 2021, 41(09): 3598-3611.
    [10] Lu K, Gao H, Yu H, et al. Insight into variations of DOM fractions in different latitudinal rural black-odor waterbodies of eastern China using fluorescence spectroscopy coupled with structure equation model[J]. Science of The Total Environment, 2021, 816.
    [11] Chen X, Chuai X, Yang L, et al. Climatic warming and overgrazing induced the high concentration of organic matter in Lake Hulun, a large shallow eutrophic steppe lake in northern China[J]. Science of The Total Environment, 2012, 431: 332-338.
    [12] 杨颖,刘吉宝,魏源送,等. 北运河沉积物中氮磷营养盐及荧光溶解性有机物的污染特征研究[J]. 环境科学学报, 2021, 1-11.
    [13] McKnight D M, Boyer E W, Westerhoff P K, et al. Spectrofluorometric characterization of dissolved organic matter for indication of precursor organic material and aromaticity[J]. Limnology and Oceanography, 2001, 46(1): 38-48.
    [14] 孙玉恒,弓晓峰,李远航,等. 不同溶解氧水平下沉积物DOM的释放及光谱特性[J]. 环境科学与技术, 2021, 44(03): 110-119.
    [15] 何杰,朱学惠,魏彬,等. 基于EEMs与UV-vis分析苏州汛期景观河道中DOM光谱特性与来源[J]. 环境科学, 2021, 42(04): 1889-1900.
    [16] 陈昭宇,李思悦. 三峡库区城镇化影响下河流DOM光谱特征季节变化[J]. 环境科学, 2021, 42(01): 195-203.
    [17] 刘纪阳,薛爽,张营,等. 水相和冰相中不同pH条件下溶解性有机质对苊光降解的影响[J]. 环境科学学报, 2021, 41(05): 1930-1939.
    [18] 高洁,江韬,李璐璐,等. 三峡库区消落带土壤中溶解性有机质(DOM)吸收及荧光光谱特征[J]. 环境科学, 2015, 36(01): 151-162.
    [19] 李卫平,滕飞,杨文焕,等. 乌梁素海冰封期冰—水中污染物空间分布特征及污染评价[J]. 灌溉排水学报, 2020, 39(02): 122-128+144.
    [20] 许冬雪,李兴,王勇,等. 冰封期乌梁素海不同形态氮、磷和叶绿素a的空间分布特征及其响应关系[J]. 生态环境学报, 2021, 30(09): 1855-1864.
    [21] 张翼鹏,文杨,薛爽,等. 水体冻结过程中荧光物质的迁移转化研究[J]. 环境科学学报, 2015, 35(06): 1710-1720.
    [22] 陈静. 水体冻结—融化过程中溶解性有机物的变化[D]. 辽宁沈阳: 辽宁大学, 2015.
    [23] 王晓云,于玲红,王非,等. 包头南海子湿地冰封期污染物迁移特征分析[J]. 环境化学, 2017, 36(04): 867-874.
    [24] 孙驰. 基于第一性原理的乌梁素海冰、水介质中重金属迁移特征研究[D]. 内蒙古呼和浩特: 内蒙古农业大学, 2019.
    [25] 孙少晨,肖伟华,于翔,等. 寒区河流冰体中污染物融出对水质的影响[J]. 南水北调与水利科技, 2015, 13(04): 664-666+680.
    [26] Choi Y, Yoon H-I, Lee C, et al. Activation of Periodate by Freezing for the Degradation of Aqueous Organic Pollutants[J]. Environmental Science Technology, 2018, 52(9): 5378-5385.
    [27] 王赫伟. 冰封期河流污染物变化规律及机理研究[D]. 辽宁沈阳: 辽宁大学, 2021.
    [28] Zhang L, Du S, Zhang X, et al. Occurrence, distribution, and ecological risk of pharmaceuticals in a seasonally ice-sealed river: From ice formation to melting[J]. Journal of Hazardous Materials, 2020, 389.
    相似文献
    引证文献
    网友评论
    网友评论
    分享到微博
    发 布
引用本文
分享
文章指标
  • 点击次数:513
  • 下载次数: 0
  • HTML阅读次数: 0
  • 引用次数: 0
历史
  • 收稿日期:2022-03-22
  • 最后修改日期:2022-05-05
  • 录用日期:2022-05-06
文章二维码