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.