垃圾填埋场地下水溶解性有机物光谱特征
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摘要
垃圾填埋为我国垃圾处理的最主要途径,填埋过程中渗滤液的泄漏将导致附近地下水污染.地下水中溶解性有机物(DOM)能示踪外来污染物的来源、形态和迁移转化过程,其组成、结构和分布的差异具有重要的环境指示意义.联合现代光谱技术及多元统计分析方法,研究了不同运行年限填埋场地下水中DOM来源、组成和分子结构特征,探究了不同年限地下水DOM动力学演化规律.结果表明,填埋场地下水DOM以微生物来源为主,其次为自生陆源.填埋前期阶段其微生物来源DOM较多,而在填埋后期微生物来源DOM减弱.填埋年限较短的填埋场地下水DOM主要为一些新生成腐殖化程度较低的易降解类色氨酸和类酪氨酸,其促进微生物活性,且各点位差异性较大,应提高预警措施.填埋时间相对较长的填埋场地下水有机质腐殖化率高,难降解的大分子物质累积,微生物活性减弱,填埋垃圾趋向稳定对地下水影响减弱.
Landfills have been the most common methods of organized waste disposal in China posing an incredible groundwater pollution threat. Dissolved organic matter( DOM) can be used to trace the source,species and migration of contaminants in groundwater,and the investigations of its composition,structure,and distribution play a role in environmental protection. This study investigated the DOM source,composition,and molecular structure in groundwater at landfills for different years of operation,and explored the dynamics of groundwater DOM evolution over time,usingmodern spectroscopy in combination with multivariate statistical analysis. The results showed that DOM in landfill groundwater was initially dominated by outputs from microbial activities,and this was followed by autogenous terrigenous input. In the early stages of landfilling,the DOM of microbial origin was significant; however,towards the late stages of landfilling,the presence of microbial DOM has weakened. The groundwater DOM with short landfill times were mainly composed of newly produced tryptophan and tyrosine,which had low humification,aromaticity,and molecular weight.Microbial activity was strong,and while there were initial,significant differences between sampling points,evidence of its presence could be used for early warning of contamination and monitoring should be conducted for its presence. Microbial activity weakened with longer landfill operation time,landfill waste tended towards stability,and the DOM in groundwater with high humification,aromaticity and molecular weight,was able to reduce the landfill impact on groundwater.
Landfills have been the most common methods of organized waste disposal in China posing an incredible groundwater pollution threat. Dissolved organic matter( DOM) can be used to trace the source,species and migration of contaminants in groundwater,and the investigations of its composition,structure,and distribution play a role in environmental protection. This study investigated the DOM source,composition,and molecular structure in groundwater at landfills for different years of operation,and explored the dynamics of groundwater DOM evolution over time,usingmodern spectroscopy in combination with multivariate statistical analysis. The results showed that DOM in landfill groundwater was initially dominated by outputs from microbial activities,and this was followed by autogenous terrigenous input. In the early stages of landfilling,the DOM of microbial origin was significant; however,towards the late stages of landfilling,the presence of microbial DOM has weakened. The groundwater DOM with short landfill times were mainly composed of newly produced tryptophan and tyrosine,which had low humification,aromaticity,and molecular weight.Microbial activity was strong,and while there were initial,significant differences between sampling points,evidence of its presence could be used for early warning of contamination and monitoring should be conducted for its presence. Microbial activity weakened with longer landfill operation time,landfill waste tended towards stability,and the DOM in groundwater with high humification,aromaticity and molecular weight,was able to reduce the landfill impact on groundwater.
引文
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[2]仝晓霞,宁立波,董少刚,等.运行GMS模型对某垃圾场地下水污染的研究[J].环境科学与技术,2012,35(7):197-201.Tong X X,Ning L B,Dong S G.GMS model for assessment and prediction of groundwater pollution of a garbage dumpling site in Luoyang[J].Environmental Science&Technology,2012,35(7):197-201.
[3]杨元丽,杨涛毅,于晓红,等.贵州岩溶地区简易垃圾填埋场对地下水的污染研究[J].地下水,2013,35(3):77-80.Yang Y L,Yang T Y,Yu X H,et al.Research on groundwater pollution caused by landfills in karst region in guizhou[J].Underground Water,2013,35(3):77-80.
[4]田扬捷,黄仁华,杨虹,等.海滨地区垃圾填埋场渗沥液对地下水系统的污染[J].环境卫生工程,2005,13(1):1-5.Tian Y J,Huang R H,Yang H,et al.Pollution on groundwater systems by the leachate from a seashore waste landfill site[J].Environmental Sanitation Engineering,2005,13(1):1-5.
[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,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,2017,42(5):771-782.
[6]Wang S L,Mulligan C N.Effect of natural organic matter on arsenic release from soils and sediments into groundwater[J].Environmental Geochemistry and Health,2006,28(3):197-214.
[7]Postma D,Larsen F,Thai N T,et al.Groundwater arsenic concentrations in Vietnam controlled by sediment age[J].Nature Geoscience,2012,5(9):656-661.
[8]郭卉,虞敏达,何小松,等.南方典型农田区浅层地下水污染特征[J].环境科学,2016,37(12):4680-4689.Guo H,Yu M D,He X S,et al.Pollution characteristics analysis in shallow groundwater of typical farmland area,southern China[J].Environmental Science,2016,37(12):4680-4689.
[9]Christensen J B,Jensen D L,Grn C,et al.Characterization of the dissolved organic carbon in landfill leachate-polluted groundwater[J].Water Research,1998,32(1):125-135.
[10]于静,虞敏达,蓝艳,等.北方典型设施蔬菜种植区地下水水质特征[J].环境科学,2017,38(9):3696-3704.Yu J,Yu M D,Lan Y,et al.Analysis of the characteristics of groundwater quality in a typical vegetable field,northern China[J].Environmental Science,2017,38(9):3696-3704.
[11]Lapworth D J,Gooddy D C,Butcher A S,et al.Tracing groundwater flow and sources of organic carbon in sandstone aquifers using fluorescence properties of dissolved organic matter(DOM)[J].Applied Geochemistry,2008,23(12):3384-3390.
[12]Bahram M,Bro R,Stedmon C,et al.Handling of Rayleigh and Raman scatter for PARAFAC modeling of fluorescence data using interpolation[J].Journal of Chemometrics,2006,20(3-4):99-105.
[13]He X S,Xi B D,Wei Z M,et al.Spectroscopic characterization of water extractable organic matter during composting of municipal solid waste[J].Chemosphere,2011,82(4):541-548.
[14]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.
[15]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.
[16]Mc Knight 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.
[17]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.
[18]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.
[19]Luo Z Y,Zhao Y C,Yuan T,et al.Natural attenuation and characterization of contaminants composition in landfill leachate under different disposing ages[J].Science of the Total Environment,2009,407(10):3385-3391.
[20]Rochelle-Newall E J,Fisher T R.Chromophoric dissolved organic matter and dissolved organic carbon in Chesapeake Bay[J].Marine Chemistry,2002,77(1):23-41.
[21]邵田田,赵莹,宋开山,等.辽河下游CDOM吸收与荧光特性的季节变化研究[J].环境科学,2014,35(10):3755-3763.Shao T T,Zhao Y,Song K S,et al.Seasonal variation in the absorption and fluorescence characteristics of CDOM in downstream of Liaohe river[J].Environmental Science,2014,35(10):3755-3763.
[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]Hur J,Kim G.Comparison of the heterogeneity within bulk sediment humic substances from a stream and reservoir via selected operational descriptors[J].Chemosphere,2009,75(4):483-490.
[24]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.
[25]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.
[26]Hua B,Dolan F,Mcghee C,et al.Water-source characterization and classification with fluorescence EEM spectroscopy:PARAFAC analysis[J].International Journal of Environmental Analytical Chemistry,2007,87(2):135-147.
[27]Kulkarni H V,Mladenov N,Johannesson K H,et al.Contrasting dissolved organic matter quality in groundwater in Holocene and Pleistocene aquifers and implications for influencing arsenic mobility[J].Applied Geochemistry,2016,77:194-205.
[28]Lu F,Chang C H,Lee D J,et al.Dissolved organic matter with multi-peak fluorophores in landfill leachate[J].Chemosphere,2009,74(4):575-582.
[29]Zhang Y L,Yin Y,Feng L Q,et al.Characterizing chromophoric dissolved organic matter in Lake Tianmuhu and its catchment basin using excitation-emission matrix fluorescence and parallel factor analysis[J].Water Research,2011,45(16):5110-5122.
[30]Coble P G.Characterization of marine and terrestrial DOM in seawater using excitation-emission matrix spectroscopy[J].Marine Chemistry,1996,51(4):325-346.
[31]He X S,Xi B D,Cui D Y,et al.Influence of chemical and structural evolution of dissolved organic matter on electron transfer capacity during composting[J].Journal of Hazardous Materials,2014,268:256-263.
[32]He X S,Xi B D,Gao R T,et al.Using fluorescence spectroscopy coupled with chemometric analysis to investigate the origin,composition,and dynamics of dissolved organic matter in leachate-polluted groundwater[J].Environmental Science and Pollution Research,2015,22(11):8499-8506.
[33]Chen M L,Price R M,Yamashita Y,et al.Comparative study of dissolved organic matter from groundwater and surface water in the Florida coastal Everglades using multi-dimensional spectrofluorometry combined with multivariate statistics[J].Applied Geochemistry,2010,25(6):872-880.
[34]Dos Santos L M,Sim7es M L,De Melo W J,et al.Application of chemometric methods in the evaluation of chemical and spectroscopic data on organic matter from Oxisols in sewage sludge applications[J].Geoderma,2010,155(1-2):121-127.
[35]Reemtsma T,Bredow A,Gehring M.The nature and kinetics of organic matter release from soil by salt solutions[J].European Journal of Soil Science,1999,50(1):53-64.
[36]Huang S B,Wang Y X,Ma T,et al.Linking groundwater dissolved organic matter to sedimentary organic matter from a fluvio-lacustrine aquifer at Jianghan Plain,China by EEMPARAFAC and hydrochemical analyses[J].Science of the Total Environment,2015,529:131-139.
[2]仝晓霞,宁立波,董少刚,等.运行GMS模型对某垃圾场地下水污染的研究[J].环境科学与技术,2012,35(7):197-201.Tong X X,Ning L B,Dong S G.GMS model for assessment and prediction of groundwater pollution of a garbage dumpling site in Luoyang[J].Environmental Science&Technology,2012,35(7):197-201.
[3]杨元丽,杨涛毅,于晓红,等.贵州岩溶地区简易垃圾填埋场对地下水的污染研究[J].地下水,2013,35(3):77-80.Yang Y L,Yang T Y,Yu X H,et al.Research on groundwater pollution caused by landfills in karst region in guizhou[J].Underground Water,2013,35(3):77-80.
[4]田扬捷,黄仁华,杨虹,等.海滨地区垃圾填埋场渗沥液对地下水系统的污染[J].环境卫生工程,2005,13(1):1-5.Tian Y J,Huang R H,Yang H,et al.Pollution on groundwater systems by the leachate from a seashore waste landfill site[J].Environmental Sanitation Engineering,2005,13(1):1-5.
[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,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,2017,42(5):771-782.
[6]Wang S L,Mulligan C N.Effect of natural organic matter on arsenic release from soils and sediments into groundwater[J].Environmental Geochemistry and Health,2006,28(3):197-214.
[7]Postma D,Larsen F,Thai N T,et al.Groundwater arsenic concentrations in Vietnam controlled by sediment age[J].Nature Geoscience,2012,5(9):656-661.
[8]郭卉,虞敏达,何小松,等.南方典型农田区浅层地下水污染特征[J].环境科学,2016,37(12):4680-4689.Guo H,Yu M D,He X S,et al.Pollution characteristics analysis in shallow groundwater of typical farmland area,southern China[J].Environmental Science,2016,37(12):4680-4689.
[9]Christensen J B,Jensen D L,Grn C,et al.Characterization of the dissolved organic carbon in landfill leachate-polluted groundwater[J].Water Research,1998,32(1):125-135.
[10]于静,虞敏达,蓝艳,等.北方典型设施蔬菜种植区地下水水质特征[J].环境科学,2017,38(9):3696-3704.Yu J,Yu M D,Lan Y,et al.Analysis of the characteristics of groundwater quality in a typical vegetable field,northern China[J].Environmental Science,2017,38(9):3696-3704.
[11]Lapworth D J,Gooddy D C,Butcher A S,et al.Tracing groundwater flow and sources of organic carbon in sandstone aquifers using fluorescence properties of dissolved organic matter(DOM)[J].Applied Geochemistry,2008,23(12):3384-3390.
[12]Bahram M,Bro R,Stedmon C,et al.Handling of Rayleigh and Raman scatter for PARAFAC modeling of fluorescence data using interpolation[J].Journal of Chemometrics,2006,20(3-4):99-105.
[13]He X S,Xi B D,Wei Z M,et al.Spectroscopic characterization of water extractable organic matter during composting of municipal solid waste[J].Chemosphere,2011,82(4):541-548.
[14]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.
[15]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.
[16]Mc Knight 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.
[17]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.
[18]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.
[19]Luo Z Y,Zhao Y C,Yuan T,et al.Natural attenuation and characterization of contaminants composition in landfill leachate under different disposing ages[J].Science of the Total Environment,2009,407(10):3385-3391.
[20]Rochelle-Newall E J,Fisher T R.Chromophoric dissolved organic matter and dissolved organic carbon in Chesapeake Bay[J].Marine Chemistry,2002,77(1):23-41.
[21]邵田田,赵莹,宋开山,等.辽河下游CDOM吸收与荧光特性的季节变化研究[J].环境科学,2014,35(10):3755-3763.Shao T T,Zhao Y,Song K S,et al.Seasonal variation in the absorption and fluorescence characteristics of CDOM in downstream of Liaohe river[J].Environmental Science,2014,35(10):3755-3763.
[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]Hur J,Kim G.Comparison of the heterogeneity within bulk sediment humic substances from a stream and reservoir via selected operational descriptors[J].Chemosphere,2009,75(4):483-490.
[24]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.
[25]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.
[26]Hua B,Dolan F,Mcghee C,et al.Water-source characterization and classification with fluorescence EEM spectroscopy:PARAFAC analysis[J].International Journal of Environmental Analytical Chemistry,2007,87(2):135-147.
[27]Kulkarni H V,Mladenov N,Johannesson K H,et al.Contrasting dissolved organic matter quality in groundwater in Holocene and Pleistocene aquifers and implications for influencing arsenic mobility[J].Applied Geochemistry,2016,77:194-205.
[28]Lu F,Chang C H,Lee D J,et al.Dissolved organic matter with multi-peak fluorophores in landfill leachate[J].Chemosphere,2009,74(4):575-582.
[29]Zhang Y L,Yin Y,Feng L Q,et al.Characterizing chromophoric dissolved organic matter in Lake Tianmuhu and its catchment basin using excitation-emission matrix fluorescence and parallel factor analysis[J].Water Research,2011,45(16):5110-5122.
[30]Coble P G.Characterization of marine and terrestrial DOM in seawater using excitation-emission matrix spectroscopy[J].Marine Chemistry,1996,51(4):325-346.
[31]He X S,Xi B D,Cui D Y,et al.Influence of chemical and structural evolution of dissolved organic matter on electron transfer capacity during composting[J].Journal of Hazardous Materials,2014,268:256-263.
[32]He X S,Xi B D,Gao R T,et al.Using fluorescence spectroscopy coupled with chemometric analysis to investigate the origin,composition,and dynamics of dissolved organic matter in leachate-polluted groundwater[J].Environmental Science and Pollution Research,2015,22(11):8499-8506.
[33]Chen M L,Price R M,Yamashita Y,et al.Comparative study of dissolved organic matter from groundwater and surface water in the Florida coastal Everglades using multi-dimensional spectrofluorometry combined with multivariate statistics[J].Applied Geochemistry,2010,25(6):872-880.
[34]Dos Santos L M,Sim7es M L,De Melo W J,et al.Application of chemometric methods in the evaluation of chemical and spectroscopic data on organic matter from Oxisols in sewage sludge applications[J].Geoderma,2010,155(1-2):121-127.
[35]Reemtsma T,Bredow A,Gehring M.The nature and kinetics of organic matter release from soil by salt solutions[J].European Journal of Soil Science,1999,50(1):53-64.
[36]Huang S B,Wang Y X,Ma T,et al.Linking groundwater dissolved organic matter to sedimentary organic matter from a fluvio-lacustrine aquifer at Jianghan Plain,China by EEMPARAFAC and hydrochemical analyses[J].Science of the Total Environment,2015,529:131-139.