城镇流域水体-沉积物中溶解性有机质的荧光特性及影响因素:以宁波市小浃江为例
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摘要
我国快速城镇化过程对流域水体和沉积物的溶解性有机质(dissolved organic matter,DOM)含量和成分产生了重要影响,探究水体-沉积物中DOM的分布特性及影响因素具有重要意义.本研究选取长三角典型城镇地区宁波市北仑区小浃江流域为研究对象,利用三维荧光光谱技术,结合PARAFAC(平行因子分析)模型及相关性分析,对小浃江流域水体及沉积物DOM光谱特性进行研究,分析DOM荧光组分特征及来源.结果表明:①小浃江水体-沉积物DOM主要包括4种组分:C1、C2、C3和C4,其中C1为陆源类腐殖质,分子量较大; C2为陆源类腐殖质,由生物降解产生,分子量较小; C3为类蛋白物质,包括类色氨酸,对微环境的变化敏感; C4为陆源类腐殖质.②小浃江水体DOM受新生内源和陆源输入共同影响,腐殖化程度较弱,腐殖质含量较低.沉积物以陆源或土壤源输入为主,内源贡献较小,DOM具有一定的腐殖化特征,腐殖质的浓度水平高于水体中腐殖质含量.③冗余分析(redundancy analysis,RDA)表明,水体DOM各组分相关性较高的环境因子主要为农田、城镇;而沉积物DOM各组分相关性较高的环境因子为城镇、农田、湿地.其中,城镇对沉积物中类腐殖质C4和类腐殖质的浓度参数Fn(355)影响最大.
Rapid urbanization has a significant impact on dissolved organic matter( DOM) in water and sediment; thus,it is important to explore the distribution characteristics and influencing factors of DOM in watersheds. Xiaojia River is a typical urban area in Beilun District of Ningbo City,Yangtze River Delta. The spectral characteristics of DOM in the water and sediment in this river were studied to examine their sources and characteristics. The DOM was analyzed by three-dimensional fluorescence spectroscopy( EEM) coupled with the parallel factor analysis( PARAFAC) model. The following results were noted. ① Four fluorescence DOM components were derived by EEM-PARAFAC: C1 represents terrestrial humus with a high molecular weight; C2 represents terrestrial humus with a low molecular weight, which was produced by biodegradation; C3 represents protein-like substances that were sensitive in a microenvironment; and C4 is terrestrial humus. ② Both new-born endogenous and terrestrial sources have large impacts on DOM components. The humification degree was very weak with a low concentration of humus. The DOM in the sediments was derived mainly from terrestrial or soil sources with small endogenous contribution with high humification. The concentration of humus in the sediments was significantly higher than that in water. ③ Redundancy analysis( RDA) showed that farmland and urban land use were the dominant environmental factors and had relatively high correlation with the water indicators. Construction land,farmland,and wetland land use positively correlated with the sediment components. Among them,urban land use had the greatest influence on the concentration parameter Fn( 355) of humus-like substance C4 and the humus-like substance in sediments.
Rapid urbanization has a significant impact on dissolved organic matter( DOM) in water and sediment; thus,it is important to explore the distribution characteristics and influencing factors of DOM in watersheds. Xiaojia River is a typical urban area in Beilun District of Ningbo City,Yangtze River Delta. The spectral characteristics of DOM in the water and sediment in this river were studied to examine their sources and characteristics. The DOM was analyzed by three-dimensional fluorescence spectroscopy( EEM) coupled with the parallel factor analysis( PARAFAC) model. The following results were noted. ① Four fluorescence DOM components were derived by EEM-PARAFAC: C1 represents terrestrial humus with a high molecular weight; C2 represents terrestrial humus with a low molecular weight, which was produced by biodegradation; C3 represents protein-like substances that were sensitive in a microenvironment; and C4 is terrestrial humus. ② Both new-born endogenous and terrestrial sources have large impacts on DOM components. The humification degree was very weak with a low concentration of humus. The DOM in the sediments was derived mainly from terrestrial or soil sources with small endogenous contribution with high humification. The concentration of humus in the sediments was significantly higher than that in water. ③ Redundancy analysis( RDA) showed that farmland and urban land use were the dominant environmental factors and had relatively high correlation with the water indicators. Construction land,farmland,and wetland land use positively correlated with the sediment components. Among them,urban land use had the greatest influence on the concentration parameter Fn( 355) of humus-like substance C4 and the humus-like substance in sediments.
引文
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[8]高凤,邵美玲,曹昌丽,等.城镇化流域氮、磷污染特征及影响因素———以宁波北仑区小浃江为例[J].湖泊科学,2019,31(3):689-699.Gao F,Shao M L,Cao C L,et al. Nitrogen and phosphorus pollution characteristics and influencing factors in urbanized watershed:a case study of Xiaojia River,Ningbo City[J].Journal of Lake Sciences,2019,31(3):689-699.
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[12]范诗雨,秦纪洪,刘堰杨,等.岷江上游水体中DOM光谱特征的季节变化[J].环境科学,2018,39(10):4530-4538.Fan S Y,Qin J H,Liu Y Y,et al. Seasonal variations of DOM spectral characteristics in the surface water of the upstream Minjiang River[J]. Environmental Science,2018,39(10):4530-4538.
[13] 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.
[14]陈俊伊,王书航,姜霞,等.蠡湖表层沉积物荧光溶解性有机质(FDOM)荧光光谱特征[J].环境科学,2017,38(1):70-77.Chen J Y,Wang S H,Jiang X,et al. Fluorescence spectral characteristics of fluorescent dissolved organic matter(FDOM)in the surface sediments from Lihu Lake[J]. Environmental Science,2017,38(1):70-77.
[15]张欢,崔康平,张强,等.派河水体中DOM的光谱分析及其来源解析[J].环境科学研究,2019,32(2):227-234.Zhang H,Cui K P,Zhang Q,et al. Spectral analysis and source analysis of dissolved organic matter in Pai River[J]. Research of Environmental Sciences,2019,32(2):227-234.
[16] Riu J,Bro R. Jack-knife technique for outlier detection and estimation of standard errors in PARAFAC models[J].Chemometrics and Intelligent Laboratory Systems,2003,65(1):35-49.
[17] Andersen C M,Bro R. Practical aspects of PARAFAC modeling of fluorescence excitation-emission data[J]. Journal of Chemometrics,2003,17(4):200-215.
[18] Bro R,Kiers H A L. A new efficient method for determining the number of components in PARAFAC models[J]. Journal of Chemometrics,2003,17(5):274-286.
[19]赵芸.溶解性天然有机质的光谱研究[D].石家庄:河北师范大学,2013. 12-36.Zhao Y. Spectroscopic study of dissolved natural organic matter[D]. Shijiazhuang:Hebei Normal University,2013. 12-36.
[20] Stedmon C A,Markager S,Bro R. Tracing dissolved organic matter in aquatic environments using a new approach to fluorescence spectroscopy[J]. Marine Chemistry,2003,82(3-4):239-254.
[21] Carstea E M,Baker A,Bieroza M,et al. Characterisation of dissolved organic matter fluorescence properties by PARAFAC analysis and thermal quenching[J]. Water Research,2014,61:152-161.
[22] Stedmon C A,Markager S. Resolving the variability in dissolved organic matter fluorescence in a temperate estuary and Its catchment using PARAFAC analysis[J]. Limnology and Oceanography,2005,50(2):686-697.
[23] Yamashita Y,Boyer J N,JafféR. Evaluating the distribution of terrestrial dissolved organic matter in a complex coastal ecosystem using fluorescence spectroscopy[J]. Continental Shelf Research,2013,66:136-144.
[24] Derrien M,Kim M S,Ock G,et al. Estimation of different source contributions to sediment organic matter in an agriculturalforested watershed using end member mixing analyses based on stable isotope ratios and fluorescence spectroscopy[J]. Science of the Total Environment,2018,618:569-578.
[25] Yamashita Y,Cory R M, Nishioka J, et al. Fluorescence characteristics of dissolved organic matter in the deep waters of the Okhotsk Sea and the northwestern North Pacific Ocean[J].Deep Sea Research Part II:Topical Studies in Oceanography,2010,57(16):1478-1485.
[26] Murphy K R,Stedmon C A,Waite T D,et al. Distinguishing between terrestrial and autochthonous organic matter sources in marine environments using fluorescence spectroscopy[J]. Marine Chemistry,2008,108(1-2):40-58.
[27] Zsolnay. Dissolved organic matter:artefacts,definitions,and functions[J]. Geoderma,2003,113(3-4):187-209.
[28] Miller M P,Mc Knight D M. Comparison of seasonal changes in fluorescent dissolved organic matter among aquatic lake and stream sites in the Green Lakes Valley[J]. Journal of Geophysical Research:Biogeosciences, 2015, 115(G1):G00F12.
[29] Kamjunke N,von Tümpling W,Hertkorn N,et al. A new approach for evaluating transformations of dissolved organic matter(DOM)via high-resolution mass spectrometry and relating it to bacterial activity[J]. Water Research,2017,123:513-523.
[30] Zheng L C, Song Z F, Meng P P, et al. Seasonal characterization and identification of dissolved organic matter(DOM)in the Pearl River,China[J]. Environmental Science and Pollution Research,2016,23(8):7462-7469.
[31]蒋愉林,黄清辉,李建华.水体有色溶解有机质的研究进展[J].江苏环境科技,2008,21(2):57-59,63.Jiang Y L, Huang Q H, Li J H. Research progress of chromophoric dissolved organic matter in nature water[J].Jiangsu Environmental Science and Technology,2008,21(2):57-59,63.
[32] 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.
[33] Zhang Y L,Zhang E L,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.
[34]梁俭,江韬,魏世强,等.夏、冬季降雨中溶解性有机质(DOM)光谱特征及来源辨析[J].环境科学,2015,36(3):888-897.Liang J,Jiang T,Wei S Q,et al. Absorption and fluorescence characteristics of dissolved organic matter(DOM)in Rainwater and sources analysis in summer and winter season[J].Environmental Science,2015,36(3):888-897.
[35]张大伟,李杨帆,孙翔,等.入太湖河流武进港的区域景观格局与河流水质相关性分析[J].环境科学,2010,31(8):1775-1783.Zhang D W, Li Y F, Sun X, et al. Relationship between landscape pattern and river water quality in Wujingang Region,Taihu Lake watershed[J]. Environmental Science,2010,31(8):1775-1783.
[36]李昀,魏鸿杰,王侃,等.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(EEMPARAFAC)[J].环境科学,2019,40(4):1751-1759.Li Y,Wei H J,Wang K,et al. Analysis of the relationship between dissolved organic matter(DOM)and watershed land-use based on three-dimensional fluorescence-parallel factor(EEMPARAFAC)analysis[J]. Environmental Science,2019,40(4):1751-1759.
[2]沈烁,王育来,杨长明,等.南淝河不同排口表层沉积物DOM光谱特征[J].中国环境科学,2014,34(9):2351-2361.Shen S,Wang Y L,Yang C M,et al. Spectral characteristic of dissolved organic matter(DOM)in the surface sediments from different discharging points along the Nanfei River in Hefei City,Anhui Province[J]. China Environmental Science,2014,34(9):2351-2361.
[3] Aiken G R,Heileen H K,Ryan J N. Influence of dissolved organic matter on the environmental fate of metals,nanoparticles,and colloids[J]. Environmental Science&Technology,2011,45(8):3196-3201.
[4] Liu E F,Shen J,Liu X Q,et al. Variation characteristics of heavy metals and nutrients in the core sediments of Taihu Lake and their pollution history[J]. Science in China Series D,2006,49(1):82-91.
[5]鲁宗杰,邓娅敏,杜尧,等.江汉平原高砷地下水中DOM三维荧光特征及其指示意义[J].地球科学-中国地质大学学报,2017,42(5):771-782.Lu Z J,Deng Y M,Du Y,et al. EEMs characteristics of dissolved organic matter and their implication in high arsenic groundwater of Jianghan Plain[J]. Earth Science-Journal of China University of Geosciences,2017,42(5):771-782.
[6]冯伟莹,焦立新,张生,等.乌梁素海沉积物溶解性有机质荧光光谱特性[J].中国环境科学,2013,33(6):1068-1074.Feng W Y,Jiao L X,Zhang S,et al. Spectral characteristics of dissolved organic matter in the sediments of Wuliangsuhai Lake[J]. China Environmental Science,2013,33(6):1068-1074.
[7]杨丽萍.浙江省两个典型流域水体污染特征及污染源解析研究[D].杭州:浙江大学,2015. 6-20.Yang L P. Water pollution characteristics and source apportionment in two representative watersheds in Zhejiang Province[D]. Hangzhang:Zhejiang University,2015. 6-20.
[8]高凤,邵美玲,曹昌丽,等.城镇化流域氮、磷污染特征及影响因素———以宁波北仑区小浃江为例[J].湖泊科学,2019,31(3):689-699.Gao F,Shao M L,Cao C L,et al. Nitrogen and phosphorus pollution characteristics and influencing factors in urbanized watershed:a case study of Xiaojia River,Ningbo City[J].Journal of Lake Sciences,2019,31(3):689-699.
[9] He W,Lee J H,Hur J. Anthropogenic signature of sediment organic matter probed by UV-Visible and fluorescence spectroscopy and the association with heavy metal enrichment[J]. Chemosphere,2016,150:184-193.
[10]曹昌丽,梁梦琦,何桂英,等.城镇化河流溶解性有机质的荧光特性与水质相关性:以宁波市北仑区芦江为例[J].环境科学,2018,39(4):1560-1567.Cao C L,Liang M Q,He G Y,et al. Fluorescent dissolved organic matter and its correlation with water quality in a urban river:a case study of the Lujiang River in Beilun,Ningbo[J].Environmental Science,2018,39(4):1560-1567.
[11] Cory R M,Mc Knight D M. Fluorescence spectroscopy reveals ubiquitous presence of oxidized and reduced quinones in dissolved organic matter[J]. Environmental Science&Technology,2005,39(21):8142-8149.
[12]范诗雨,秦纪洪,刘堰杨,等.岷江上游水体中DOM光谱特征的季节变化[J].环境科学,2018,39(10):4530-4538.Fan S Y,Qin J H,Liu Y Y,et al. Seasonal variations of DOM spectral characteristics in the surface water of the upstream Minjiang River[J]. Environmental Science,2018,39(10):4530-4538.
[13] 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.
[14]陈俊伊,王书航,姜霞,等.蠡湖表层沉积物荧光溶解性有机质(FDOM)荧光光谱特征[J].环境科学,2017,38(1):70-77.Chen J Y,Wang S H,Jiang X,et al. Fluorescence spectral characteristics of fluorescent dissolved organic matter(FDOM)in the surface sediments from Lihu Lake[J]. Environmental Science,2017,38(1):70-77.
[15]张欢,崔康平,张强,等.派河水体中DOM的光谱分析及其来源解析[J].环境科学研究,2019,32(2):227-234.Zhang H,Cui K P,Zhang Q,et al. Spectral analysis and source analysis of dissolved organic matter in Pai River[J]. Research of Environmental Sciences,2019,32(2):227-234.
[16] Riu J,Bro R. Jack-knife technique for outlier detection and estimation of standard errors in PARAFAC models[J].Chemometrics and Intelligent Laboratory Systems,2003,65(1):35-49.
[17] Andersen C M,Bro R. Practical aspects of PARAFAC modeling of fluorescence excitation-emission data[J]. Journal of Chemometrics,2003,17(4):200-215.
[18] Bro R,Kiers H A L. A new efficient method for determining the number of components in PARAFAC models[J]. Journal of Chemometrics,2003,17(5):274-286.
[19]赵芸.溶解性天然有机质的光谱研究[D].石家庄:河北师范大学,2013. 12-36.Zhao Y. Spectroscopic study of dissolved natural organic matter[D]. Shijiazhuang:Hebei Normal University,2013. 12-36.
[20] Stedmon C A,Markager S,Bro R. Tracing dissolved organic matter in aquatic environments using a new approach to fluorescence spectroscopy[J]. Marine Chemistry,2003,82(3-4):239-254.
[21] Carstea E M,Baker A,Bieroza M,et al. Characterisation of dissolved organic matter fluorescence properties by PARAFAC analysis and thermal quenching[J]. Water Research,2014,61:152-161.
[22] Stedmon C A,Markager S. Resolving the variability in dissolved organic matter fluorescence in a temperate estuary and Its catchment using PARAFAC analysis[J]. Limnology and Oceanography,2005,50(2):686-697.
[23] Yamashita Y,Boyer J N,JafféR. Evaluating the distribution of terrestrial dissolved organic matter in a complex coastal ecosystem using fluorescence spectroscopy[J]. Continental Shelf Research,2013,66:136-144.
[24] Derrien M,Kim M S,Ock G,et al. Estimation of different source contributions to sediment organic matter in an agriculturalforested watershed using end member mixing analyses based on stable isotope ratios and fluorescence spectroscopy[J]. Science of the Total Environment,2018,618:569-578.
[25] Yamashita Y,Cory R M, Nishioka J, et al. Fluorescence characteristics of dissolved organic matter in the deep waters of the Okhotsk Sea and the northwestern North Pacific Ocean[J].Deep Sea Research Part II:Topical Studies in Oceanography,2010,57(16):1478-1485.
[26] Murphy K R,Stedmon C A,Waite T D,et al. Distinguishing between terrestrial and autochthonous organic matter sources in marine environments using fluorescence spectroscopy[J]. Marine Chemistry,2008,108(1-2):40-58.
[27] Zsolnay. Dissolved organic matter:artefacts,definitions,and functions[J]. Geoderma,2003,113(3-4):187-209.
[28] Miller M P,Mc Knight D M. Comparison of seasonal changes in fluorescent dissolved organic matter among aquatic lake and stream sites in the Green Lakes Valley[J]. Journal of Geophysical Research:Biogeosciences, 2015, 115(G1):G00F12.
[29] Kamjunke N,von Tümpling W,Hertkorn N,et al. A new approach for evaluating transformations of dissolved organic matter(DOM)via high-resolution mass spectrometry and relating it to bacterial activity[J]. Water Research,2017,123:513-523.
[30] Zheng L C, Song Z F, Meng P P, et al. Seasonal characterization and identification of dissolved organic matter(DOM)in the Pearl River,China[J]. Environmental Science and Pollution Research,2016,23(8):7462-7469.
[31]蒋愉林,黄清辉,李建华.水体有色溶解有机质的研究进展[J].江苏环境科技,2008,21(2):57-59,63.Jiang Y L, Huang Q H, Li J H. Research progress of chromophoric dissolved organic matter in nature water[J].Jiangsu Environmental Science and Technology,2008,21(2):57-59,63.
[32] 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.
[33] Zhang Y L,Zhang E L,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.
[34]梁俭,江韬,魏世强,等.夏、冬季降雨中溶解性有机质(DOM)光谱特征及来源辨析[J].环境科学,2015,36(3):888-897.Liang J,Jiang T,Wei S Q,et al. Absorption and fluorescence characteristics of dissolved organic matter(DOM)in Rainwater and sources analysis in summer and winter season[J].Environmental Science,2015,36(3):888-897.
[35]张大伟,李杨帆,孙翔,等.入太湖河流武进港的区域景观格局与河流水质相关性分析[J].环境科学,2010,31(8):1775-1783.Zhang D W, Li Y F, Sun X, et al. Relationship between landscape pattern and river water quality in Wujingang Region,Taihu Lake watershed[J]. Environmental Science,2010,31(8):1775-1783.
[36]李昀,魏鸿杰,王侃,等.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(EEMPARAFAC)[J].环境科学,2019,40(4):1751-1759.Li Y,Wei H J,Wang K,et al. Analysis of the relationship between dissolved organic matter(DOM)and watershed land-use based on three-dimensional fluorescence-parallel factor(EEMPARAFAC)analysis[J]. Environmental Science,2019,40(4):1751-1759.
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