冰体融化过程中三线态溶解性有机物的释放规律

李旭; 薛爽; 于英潭; 姜彩虹; 刘强

doi:10.13205/j.hjgc.202403005

冰体融化过程中三线态溶解性有机物的释放规律

doi: 10.13205/j.hjgc.202403005

辽宁大学环境学院, 沈阳 110036

基金项目:

国家自然科学基金项目(41771503)

详细信息

作者简介:
李旭(1997-),女,硕士研究生,主要研究方向为低温条件下污染物的环境行为。2514299948@qq.com

通讯作者:
薛爽(1977-),女,博士,教授,主要研究方向为低温条件下污染物的环境行为。xueshuang666@sina.com

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- 被引次数: 0
出版历程
- 收稿日期: 2023-02-08
- 网络出版日期: 2024-05-31

RELEASE LAW OF TRIPLET STATES OF DISSOLVED ORGANIC MATTER DURING ICE MELTING PROCESS

School of Environmental Science, Liaoning University, Shenyang 110036, China

摘要

摘要: 以辽宁省沈阳市的浑河河水(HR)和丁香湖湖水(DXL)作为研究对象,通过淋溶实验和室内模拟光解实验,选用2,4,6-三甲基苯酚(TMP)作为三线态溶解性有机物(³DOM^*)的探针,考察了不同温度条件下冰体融化时溶解性有机物(DOM)的光谱学特性变化,以及DOM、荧光物质和³DOM^*的释放规律。结果表明:融化温度越低,HR与DXL 2种水样的SUVA₂₅₄、E₂/E₃均显著增加,且DXL水样表现出的增加更为明显。HR和DXL水样中均包含类富里酸类物质、类腐植酸类物质,HR样品中还含有类芳香族蛋白类物质。冻结温度相同,融化温度越低,荧光物质从样品中析出得越规律,呈逐渐减少的趋势。融化温度越低,³DOM^*的释放越规律,且HR表现得尤为明显,HR融化初期³DOM^*的稳态浓度是原始水样的4.1倍。
- 三线态溶解性有机物 /
- 2,4,6-三甲基苯酚(TMP) /
- 三维荧光光谱 /
- 光谱学特性参数 /
- 冰体融化
Abstract: The water of Hun River (HR) and Dingxiang Lake (DXL) in Shenyang City, Liaoning Province was selected as the research objects, the changes in spectral properties of dissolved organic matter (DOM), as well as the release of DOM, fluorescent matter, and the triplet states of dissolved organic matter (³DOM^*) during ice melting process at different temperatures were investigated in this study. The leaching experiments and laboratory simulation photolysis experiments were conducted, and 2, 4, 6-trimethylphenol (TMP) was selected as the probe of ³DOM^*. The results showed that the lower the melting temperature, the SUVA₂₅₄, E₂/E₃ of the two water samples increased significantly, and the increase of DXL was more obvious. HR and DXL samples both contain fulvic acid and humic acid substances, and HR samples also contain aromatic protein substances. With the same freezing temperature, the lower the melting temperature, the more regular the precipitation of fluorescent substances from the sample, showing a gradually decreasing trend. The lower the melting temperature, the more regular the release of ³DOM^*, which was particularly obvious for HR. The steady-state concentration of ³DOM^* at the initial melting stage of HR was 4.1 times that of the original water sample.

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参考文献(39)

[1]	BRIMBLECOMBE P, CLEGG S L, DAVIES T D, et al.Observations of the preferential loss of major ions from melting snow and laboratory ice[J]. Water Research,1987,21(10):1279-1286.
[2]	BRIMBLECOMBE P, CLEGG S L, DAVIES T D, et al. The loss of halide and sulphate ions from melting ice[J]. Water Research,1988,22(6):693-700.
[3]	李宁. 溶解性有机质对羟基自由基氧化降解有机污染物的影响[D].大连:大连理工大学,2015.
[4]	WANG J Q, WANG K, GUO Y C, et al. Photochemical degradation of nebivolol in different natural organic matter solutions under simulated sunlight irradiation:kinetics, mechanism and degradation pathway[J]. Water Research,2020,173(C):115524.
[5]	CHEN Q C, MU Z, XU L, et al. Triplet-state organic matter in atmospheric aerosols:formation characteristics and potential effects on aerosol aging[J]. Atmospheric Environment,2021,252:118343.
[6]	白凯,君珊,郑朔方,等.呼伦湖水体溶解性有机物荧光特征及来源分析[J/OL].环境工程技术学报:1-14[2023-01-18 ].http://zz.xue1888.com/kcms/detail/11.5972.X.20220711.1651.006.html.
[7]	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(4):1889-1900.
[8]	周石磊,孙悦,张艺冉,等.周村水库四季变化过程中水体溶解性有机物的分布与光谱特征[J].环境科学学报,2019,39(10):3492-3502.
[9]	ZHOU X, MOPPER K. Determination of photochemically produced hydroxyl radicals in seawater and freshwater[J]. Marine Chemistry,1990,30.
[10]	COOPER W J, ZIKA R G, PETASNE R G, et al. Photochemical formation of hydrogen peroxide in natural waters exposed to sunlight[J]. Environmental Science & Technology,1988,22(4598):711-712.
[11]	HOU Z C, FANG Q, LIU H Y, et al. Photolytic kinetics of pharmaceutically active compounds from upper to lower estuarine waters:roles of triplet-excited dissolved organic matter and halogen radicals[J]. Environmental Pollution,2021,276:116692.
[12]	BRACCHINI L, LOISELLE S, DATTILO A M, et al. The spatial distribution of optical properties in the ultraviolet and visible in an aquatic ecosystem[J]. Photochemistry and photobiology,2004,80(1):139-149.
[13]	ELISA DE L, MARCO M, VALTER M, et al. Photochemical production of organic matter triplet states in water samples from mountain lakes, located below or above the tree line[J]. Chemosphere,2012,88(10):1208-1213.
[14]	陈彦彤,李旭东,陶冶,等.有机激发三重态参与的光化学反应研究进展[J].化工进展,2020,39(8):3344-3353.
[15]	闫晓寒,韩璐,文威,等.辽河保护区水体溶解性有机质空间分布与来源解析[J].环境科学学报, 2021, 41(4):1419-1427.
[16]	王杰琼. 近岸海水中溶解性有机质对有机微污染物光降解行为的影响[D].大连:大连理工大学,2019.
[17]	郭忠禹. 海水溶解性有机质对磺胺氯哒嗪光降解的影响[D]. 大连:大连理工大学,2020.
[18]	苏欣颖,王宇,程欣,等.哈尔滨市降雪中溶解性有机物光谱特性分析[J].环境化学,2021,40(1):312-320.
[19]	陈静. 水体冻结-融化过程中溶解性有机物的变化[D].沈阳:辽宁大学,2015.
[20]	XUE S, CHEN J, TIE M. Release of dissolved organic matter from melting ice[J]. Environmental Progress & Sustainable Energy,2016,35(5):1458-1467.
[21]	WENK J, GRAF C, AESCHBACHER M, et al. Effect of solution pH on the dual role of dissolved organic matter in sensitized pollutant photooxidation[J]. Environmental Science & Technology, 2021,55(22):15110-15122.
[22]	PEURAWORI J, PIHLAJA K. Molecular size distribution and spectroscopic properties of aquatic humic substances[J]. Analytica Chimica Acta,1997,337(2):133-149.
[23]	YANG C H, LIU Y Z, ZHU Y X,et al. Insights into the binding interactions of autochthonous dissolved organic matter released from Microcystis aeruginosa with pyrene using spectroscopy[J]. Marine Pollution Bulletin,2016,104(1/2):113-120.
[24]	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(5):1930-1939.
[25]	CHEN M L, MAIE N, PARISH K, et al. Spatial and temporal variability of dissolved organic matter quantity and composition in an oligotrophic subtropical coastal wetland[J]. Biogeochemistry, 2013, 115(1):167-183.
[26]	DIANE M M, ELIZABETH W B, PAUL K W, et al. Spectrofluorometric characterization of dissolved organic matter for indication of precursor organic material and aromaticity[J]. Limnology and Oceanography,2001,46(1). DOI: 10.4319/L0.2001.46.1.0038.
[27]	JUSTIN E B, ANNETTE S E. Characterization of dissolved organic matter in cave and spring waters using UV-Vis absorbance and fluorescence spectroscopy[J]. Organic Geochemistry,2009,41(3):270-280.
[28]	孟永霞,程艳,李琳,等.新疆匹里青河小流域DOM荧光特征及与汞的相互作用[J].生态与农村环境学报,2020,36(6):770-777.
[29]	JAFFÉ R, BOYER J N, LU X,et al. Source characterization of dissolved organic matter in a subtropical mangrove-dominated estuary by fluorescence analysis[J]. Marine Chemistry,2003,84(3/4):195-210.
[30]	ZHANG Y, ZHANG E, YIN Y, et al. Characteristics and sources of chromophoric dissolved organic matter in lakes of the Yungui Plateau, China, differing in trophic state and altitude[J]. Limnology and Oceanography,2010,55(6):2645-2659.
[31]	CHEN W,WESTERHOFF P,LEENHEER J A,et al. Fluorescence excitation-emission matrix regional integration to quantify spectra for dissolved organic matter[J]. Environmental Science & Technology,2003,37(24):5701-5710.
[32]	WU F C, TANOUE E, LIU C Q. Fluorescence and amino acid characteristics of molecular size fractions of DOM in the waters of Lake Biwa[J]. Biogeochemistry,2003,65(2):245-257.
[33]	NIETO-CID M, ÁLVAREZ-SALGADO X A, PÉREZ F F. Microbial and photochemical reactivity of fluorescent dissolved organic matter in a coastal upwelling system[J]. Limnology and Oceanography,2006,51(3):1391-1400.
[34]	KRAMER G D, HERNDL G J. Photo- and bioreactivity of chromophoric dissolved organic matter produced by marine bacterioplankton[J]. Aquatic Microbial Ecology,2004,36(3):239-246.
[35]	WANG H, WANG Y H, ZHUANG W, et al. Effects of fish culture on particulate organic matter in a reservoir-type river as revealed by absorption spectroscopy and fluorescence EEM-PARAFAC[J]. Chemosphere,2020,239(C):124734.
[36]	MEGHAN O'CONNOR, SAMANTHA R H, DOUGLAS E L, et al. Quantifying photo-production of triplet excited states and singlet oxygen from effluent organic matter[J]. Water Research,2019,156:23-33.
[37]	郭晗,关雪峰,薛爽,等.光照条件下冰相中激发三线态溶解性有机物的生成及其对三甲基苯酚的光敏化降解作用[J].环境科学学报,2022,42(8):186-193.
[38]	GLOVER C M, ROSARIO-ORTIZ F L. Impact of halides on the photoproduction of reactive intermediates from organic matter[J]. Environmental Science & Technology,2013,47(24):13949-13956.
[39]	MCCABE A J, ARNOLD W A. Reactivity of triplet excited states of dissolved natural organic matter in stormflow from mixed-use watersheds[J]. Environmental Science Technology,2017,51(17):9718-9728.