溶解性有机物(DOM)与区域土地利用的关系:基于三维荧光-平行因子分析(EEM-PARAFAC)
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摘要
溶解性有机物(DOM)是水体质量的综合性指标,反映了流域内经济发展和治理保护等多方面因素,可为流域水体保护提供依据.本研究采集了宁波市4个不同城市化程度的区域内的河流样本,运用三维荧光结合平行因子分析法(EEMPARAFAC)对水体中DOM进行解析,探讨了区域土地利用与DOM的关系.结果表明城市化在含量和组成两方面影响了流域水体中DOM的特征.城市区域(DOC=3. 18 mg·L~(-1))和城乡结合区域(DOC=7. 45 mg·L~(-1))水体中DOM的浓度远高于城市化程度较低的农村区域(DOC为2. 16～2. 62 mg·L~(-1),ANOVA,P <0. 001). EEM-PARAFAC解析得到7个荧光组分,主要可归为类腐殖质和类蛋白质类物质.其中,城市区域DOM以类腐殖质物质为主,占比达到61. 3%;而城乡结合区域由于受到更多的生活污水排放影响,类蛋白质物质的比例最高为59. 4%;相比之下,农村区域虽然DOM浓度相对较低,但类腐殖质物质占比达63. 6%～65. 7%,面源污染是主要原因.主成分分析表明城市化发展对水质具有重要影响,在城市化初期污染主要来源于生活和工业污染源,当城市化到一定水平污染物更多来源于路面径流.本研究表明EEM-PARAFAC可以半定量辨析水体污染源,可为不同的区域水质恢复与治水策略制定提供针对性数据支撑.
Dissolved organic matter( DOM) is a characteristic index of water quality,and reflects many factors,such as the economic development and protection policies of watershed. In this study,surface water samples were collected from four watersheds with different levels of urbanization in Ningbo. The DOM was analyzed using an excitation-emission matrix combined with parallel factor analysis( EEM-PARAFAC) to explore the relationship between land-use and DOM. The results show that the urbanization level affected both the amount and the composition of the DOM in the studied watersheds. The concentrations of DOM evaluated by dissolved organic carbon( DOC) in urban areas( DOC = 3. 18 mg·L~(-1)) and an urban-rural combined area( DOC = 7. 45 mg·L~(-1)) were much higher than those in rural areas with low urbanization( DOC between 2. 16 and 2. 62 mg·L~(-1),ANOVA,P < 0. 001). A total of seven PARAFAC components were identified in the studied watersheds,mainly including humic-like and protein-like substances. In the highly urbanized area,DOM was mainly composed of humic-like substances,with a proportion of 61. 3%. However,the water samples from the urban-rural combined area exhibited a high proportion( 59. 4%) of protein-like substances,indicating a strong influence of sewage and industrial discharge. In contrast,although the DOM amounts in rural areas were relatively low,the proportions of humuslike substances were high,ranging from 63. 6% to 65. 7%. Agricultural non-point sources were the main contributor to DOM in these areas. Moreover,the results suggest that the urbanization process could intensify the damage to the surface waters. At the initial stage of urbanization( i. e.,urban-rural combined area),contaminants are mainly discharged from sewage and industrial sources; when urbanization reaches a certain level,e. g.,with a well-constructed sewage collection system,water contaminants originate more from surface runoff rather than sewage. The results of this study suggest that the EEM-PARAFAC technique can provide semi-quantitative source tracking of surface water,as well as an inexpensive and effective tool for policy makers to overcome the insensitivity of general water quality indices.
Dissolved organic matter( DOM) is a characteristic index of water quality,and reflects many factors,such as the economic development and protection policies of watershed. In this study,surface water samples were collected from four watersheds with different levels of urbanization in Ningbo. The DOM was analyzed using an excitation-emission matrix combined with parallel factor analysis( EEM-PARAFAC) to explore the relationship between land-use and DOM. The results show that the urbanization level affected both the amount and the composition of the DOM in the studied watersheds. The concentrations of DOM evaluated by dissolved organic carbon( DOC) in urban areas( DOC = 3. 18 mg·L~(-1)) and an urban-rural combined area( DOC = 7. 45 mg·L~(-1)) were much higher than those in rural areas with low urbanization( DOC between 2. 16 and 2. 62 mg·L~(-1),ANOVA,P < 0. 001). A total of seven PARAFAC components were identified in the studied watersheds,mainly including humic-like and protein-like substances. In the highly urbanized area,DOM was mainly composed of humic-like substances,with a proportion of 61. 3%. However,the water samples from the urban-rural combined area exhibited a high proportion( 59. 4%) of protein-like substances,indicating a strong influence of sewage and industrial discharge. In contrast,although the DOM amounts in rural areas were relatively low,the proportions of humuslike substances were high,ranging from 63. 6% to 65. 7%. Agricultural non-point sources were the main contributor to DOM in these areas. Moreover,the results suggest that the urbanization process could intensify the damage to the surface waters. At the initial stage of urbanization( i. e.,urban-rural combined area),contaminants are mainly discharged from sewage and industrial sources; when urbanization reaches a certain level,e. g.,with a well-constructed sewage collection system,water contaminants originate more from surface runoff rather than sewage. The results of this study suggest that the EEM-PARAFAC technique can provide semi-quantitative source tracking of surface water,as well as an inexpensive and effective tool for policy makers to overcome the insensitivity of general water quality indices.
引文
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[31] Zhao H X,Jiang X W,Dong Y W,et al. Geographic information system-based optimization of sewage treatment facilities by evaluating pollution effects and governance demands[J]. Journal of Water Reuse and Desalination,2015,5(2):104-118.
[32]宋亚丽,王奇梁,董秉直,等.微污染水源水中有机物的分布特征及微滤膜对其的影响作用[J].环境科学学报,2016,36(10):3623-3628.Song Y L, Wang Q L, Dong B Z, et al. Distribution characteristics of organic matters in micro-polluted water and variation after microfiltration[J]. Acta Scientiae Circumstantiae,2016,36(10):3623-3628.
[33] Altmann J,Massa L,Sperlich A,et al. UV254absorbance as real-time monitoring and control parameter for micropollutant removal in advanced wastewater treatment with powdered activated carbon[J]. Water Research,2016,94:240-245.
[34] Murphy K R, Hambly A, Singh S, et al. Organic matter fluorescence in municipal water recycling schemes:toward a unified PARAFAC model[J]. Environmental Science&Technology,2011,45(7):2909-2916.
[35] Ohno T,Fernandez I J,Hiradate S,et al. Effects of soil acidification and forest type on water soluble soil organic matter properties[J]. Geoderma,2007,140(1-2):176-187.
[36] Wu F C,Evans R D,Dillon P J. Separation and characterization of NOM by high-performance liquid chromatography and on-line three-dimensional excitation emission matrix fluorescence detection[J]. Environmental Science&Technology,2003,37(16):3687-3693.
[37] Zhao C,Wang C C,Li J Q,et al. Dissolved organic matter in urban stormwater runoff at three typical regions in Beijing:chemical composition, structural characterization and source identification[J]. RSC Advances, 2015, 5(90):73490-73500.
[38] Lapierre J F,Del Giorgio P A. Partial coupling and differential regulation of biologically and photochemically labile dissolved organic carbon across boreal aquatic networks[J].Biogeosciences,2014,11(20):5969-5985.
[39] Yamashita Y,Tanoue E. Chemical characterization of proteinlike fluorophores in DOM in relation to aromatic amino acids[J].Marine Chemistry,2003,82(3-4):255-271.
[40] Mayer L M,Schick L L,LoderⅢT C. Dissolved protein fluorescence in two Maine estuaries[J]. Marine Chemistry,1999,64(3):171-179.
[41] Yan S W,Yao B,Lian L S,et al. Development of fluorescence surrogates to predict the photochemical transformation of pharmaceuticals in wastewater effluents[J]. Environmental Science&Technology,2017,51(5):2738-2747.
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[2] Cheng X,Chen L D,Sun R H,et al. Land use changes and socio-economic development strongly deteriorate river ecosystem health in one of the largest basins in China[J]. Science of the Total Environment,2018,616-617:376-385.
[3] Meng F G,Huang G C,Yang X,et al. Identifying the sources and fate of anthropogenically impacted dissolved organic matter(DOM)in urbanized rivers[J]. Water Research,2013,47(14):5027-5039.
[4]石效卷,李璐,张涛.水十条水实条——对《水污染防治行动计划》的解读[J].环境保护科学,2015,41(3):1-3.Shi X J,Li L,Zhang T. Water pollution control action plan,a realistic and pragmatic plan——an interpretation of water pollution control action plan[J]. Environmental Protection Science,2015,41(3):1-3.
[5]姜斌.对河长制管理制度问题的思考[J].中国水利,2016,(21):6-7.Jiang B. Considerations for leader responsible system in governance of rivers and lakes[J]. China Water Resources,2016,(21):6-7.
[6]刘国锋,包先明,吴婷婷,等.水葫芦生态工程措施对太湖竺山湖水环境修复效果的研究[J].农业环境科学学报,2015,34(2):352-360.Liu G F,Bao X M,Wu T T,et al. Purification of water in Zhushan bay of Taihu Lake with water hyacinth ecological engineering[J]. Journal of Agro-Environment Science,2015,34(2):352-360.
[7] Lee J,Lee S,Yu S,et al. Relationships between water quality parameters in rivers and lakes:BOD5,COD,NBOPs,and TOC[J]. Environmental Monitoring and Assessment,2016,188(4):252.
[8]杜慧玲,于晓英,曲茉莉.松花江干流哈尔滨段COD和氨氮动态水环境容量研究[J].水资源与水工程学报,2018,29(2):69-75,83.Du H L,Yu X Y,Qu M L. Research on COD and NH3-N dynamic environmental capacity in Harbin section of the Songhua River[J]. Journal of Water Resources and Water Engineering,2018,29(2):69-75,83.
[9]庆旭瑶,任玉芬,吕志强,等.重庆市主城区次级河流总氮总磷污染特征分析及富营养化评价[J].环境科学,2015,36(7):2446-2452.Qing X Y,Ren Y F,LüZ Q,et al. Characteristics of total nitrogen and total phosphorus pollution and eutrophication assessment of secondary river in urban Chongqing[J].Environmental Science,2015,36(7):2446-2452.
[10] Wang S R,Jin X C,Yan P,et al. Phosphorus fractions and phosphate sorption characteristics in relation to the sediment compositions of shallow lakes in the middle and lower reaches of Yangtze River region,China[J]. Journal of Colloid and Interface Science,2005,289(2):339-346.
[11] Cheng X,Chen L D,Sun R H,et al. An improved export coefficient model to estimate non-point source phosphorus pollution risks under complex precipitation and terrain conditions[J]. Environmental Science and Pollution Research,2018,25(21):20946-20955.
[12]李昂,李晔,成唯,等.汤逊湖流域农业面源氮、磷入湖通量计算[J].环境科学与技术,2016,39(10):113-117.Li A,Li Y,Cheng W,et al. Calculation of agricultural nonpoint source of nitrogen and phosphorus loading from Tangxun lake watershed into the lake[J]. Environmental Science&Technology,2016,39(10):113-117.
[13] Guo W D,Xu J,Wang J P,et al. Characterization of dissolved organic matter in urban sewage using excitation emission matrix fluorescence spectroscopy and parallel factor analysis[J]. Journal of Environmental Sciences,2010,22(11):1728-1734.
[14] Vera M,Cruz S,Boleda M R,et al. Fluorescence spectroscopy and parallel factor analysis as a dissolved organic monitoring tool to assess treatment performance in drinking water trains[J].Science of the Total Environment, 2017, 584-585:1212-1220.
[15] Stedmon C A,Bro R. Characterizing dissolved organic matter fluorescence with parallel factor analysis:a tutorial[J].Limnology and Oceanography Methods,2008,6(11):572-579.
[16] Hosen J D,Mc Donough O T,Febria C M,et al. Dissolved organic matter quality and bioavailability changes across an urbanization gradient in headwater streams[J]. Environmental Science&Technology,2014,48(14):7817-7824.
[17] Nimptsch J,Woelfl S,Osorio S,et al. Tracing dissolved organic matter(DOM)from land-based aquaculture systems in North Patagonian streams[J]. Science of the Total Environment,2015,537:129-138.
[18] Williams C J,Yamashita Y,Wilson H F,et al. Unraveling the role of land use and microbial activity in shaping dissolved organic matter characteristics in stream ecosystems[J].Limnology and Oceanography,2010,55(3):1159-1171.
[19] Fellman J B,Hood E,Edwards R T,et al. Changes in the concentration, biodegradability, and fluorescent properties of dissolved organic matter during stormflows in coastal temperate watersheds[J]. Journal of Geophysical Research,2009,114(G1):G01021.
[20] Yamashita Y,JafféR,Maie N,et al. Assessing the dynamics of dissolved organic matter(DOM)in coastal environments by excitation emission matrix fluorescence and parallel factor analysis(EEM-PARAFAC)[J]. Limnology and Oceanography,2008,53(5):1900-1908.
[21] Fellman J B,Miller M P,Cory R M,et al. Characterizing dissolved organic matter using PARAFAC modeling of fluorescence spectroscopy:a comparison of two models[J]. Environmental Science&Technology,2009,43(16):6228-6234.
[22] Fellman J B, Hood E, Spencer R G M. Fluorescence spectroscopy opens new windows into dissolved organic matter dynamics in freshwater ecosystems:a review[J]. Limnology and Oceanography,2010,55(6):2452-2462.
[23] Yang X L,Yu X B,Cheng J R,et al. Impacts of land-use on surface waters at the watershed scale in southeastern China:insight from fluorescence excitation-emission matrix and PARAFAC[J]. Science of the Total Environment,2018,627:647-657.
[24] Pifer A D,Fairey J L. Improving on SUVA254using fluorescencePARAFAC analysis and asymmetric flow-field flow fractionation for assessing disinfection byproduct formation and control[J].Water Research,2012,46(9):2927-2936.
[25] Weishaar J L,Aiken G R,Bergamaschi B A,et al. Evaluation of specific ultraviolet absorbance as an indicator of the chemical composition and reactivity of dissolved organic carbon[J].Environmental Science&Technology,2003,37(20):4702-4708.
[26] Helms J R,Stubbins A,Ritchie J D,et al. Absorption spectral slopes and slope ratios as indicators of molecular weight,source,and photobleaching of chromophoric dissolved organic matter[J].Limnology and Oceanography,2008,53(3):955-969.
[27] Zsolnay A,Baigar E,Jimenez M,et al. Differentiating with fluorescence spectroscopy the sources of dissolved organic matter in soils subjected to drying[J]. Chemosphere,1999,38(1):45-50.
[28] Huguet A,Vacher L,Relexans S,et al. Properties of fluorescent dissolved organic matter in the Gironde Estuary[J]. Organic Geochemistry,2009,40(6):706-719.
[29] Wilson H F,Xenopoulos M A. Effects of agricultural land use on the composition of fluvial dissolved organic matter[J]. Nature Geoscience,2009,2(1):37-41.
[30] Bhattacharya R, Osburn C L. Multivariate analyses of phytoplankton pigment fluorescence from a freshwater river network[J]. Environmental Science&Technology,2017,51(12):6683-6690.
[31] Zhao H X,Jiang X W,Dong Y W,et al. Geographic information system-based optimization of sewage treatment facilities by evaluating pollution effects and governance demands[J]. Journal of Water Reuse and Desalination,2015,5(2):104-118.
[32]宋亚丽,王奇梁,董秉直,等.微污染水源水中有机物的分布特征及微滤膜对其的影响作用[J].环境科学学报,2016,36(10):3623-3628.Song Y L, Wang Q L, Dong B Z, et al. Distribution characteristics of organic matters in micro-polluted water and variation after microfiltration[J]. Acta Scientiae Circumstantiae,2016,36(10):3623-3628.
[33] Altmann J,Massa L,Sperlich A,et al. UV254absorbance as real-time monitoring and control parameter for micropollutant removal in advanced wastewater treatment with powdered activated carbon[J]. Water Research,2016,94:240-245.
[34] Murphy K R, Hambly A, Singh S, et al. Organic matter fluorescence in municipal water recycling schemes:toward a unified PARAFAC model[J]. Environmental Science&Technology,2011,45(7):2909-2916.
[35] Ohno T,Fernandez I J,Hiradate S,et al. Effects of soil acidification and forest type on water soluble soil organic matter properties[J]. Geoderma,2007,140(1-2):176-187.
[36] Wu F C,Evans R D,Dillon P J. Separation and characterization of NOM by high-performance liquid chromatography and on-line three-dimensional excitation emission matrix fluorescence detection[J]. Environmental Science&Technology,2003,37(16):3687-3693.
[37] Zhao C,Wang C C,Li J Q,et al. Dissolved organic matter in urban stormwater runoff at three typical regions in Beijing:chemical composition, structural characterization and source identification[J]. RSC Advances, 2015, 5(90):73490-73500.
[38] Lapierre J F,Del Giorgio P A. Partial coupling and differential regulation of biologically and photochemically labile dissolved organic carbon across boreal aquatic networks[J].Biogeosciences,2014,11(20):5969-5985.
[39] Yamashita Y,Tanoue E. Chemical characterization of proteinlike fluorophores in DOM in relation to aromatic amino acids[J].Marine Chemistry,2003,82(3-4):255-271.
[40] Mayer L M,Schick L L,LoderⅢT C. Dissolved protein fluorescence in two Maine estuaries[J]. Marine Chemistry,1999,64(3):171-179.
[41] Yan S W,Yao B,Lian L S,et al. Development of fluorescence surrogates to predict the photochemical transformation of pharmaceuticals in wastewater effluents[J]. Environmental Science&Technology,2017,51(5):2738-2747.
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