西宁近郊大气氮干湿沉降研究
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摘要
本研究在青海省西宁市城郊二十里铺莫家泉湾气象站开展了完整的2年(2014和2015年)大气无机氮干沉降和混合沉降(湿沉降加部分干沉降)监测.干沉降估算通过被动采样器采集的NH_3和NO_2浓度和Geos-Chem全球化学模式模拟的气体干沉降速率相乘获得;混合沉降的测定采用雨量器.结果表明,气态NH_3和NO_2年均浓度分别为8.8μg·m-3和19.6μg·m-3,且2015年NH_3月均浓度显著高于2014年.NH_3浓度的季节变化呈现春夏高、秋冬低的特征,而NO_2浓度季节变化幅度较小.降水中NH_4~+-N和NO-3-N年均浓度为2.2 mg·L~(-1)和1.8 mg·L~(-1),秋季降水NH_4~+-N浓度比其他季节低55%,而NO-3-N浓度在秋冬季比春夏季高约26%.气态NH_3和NO_2的干沉降量分别为9.0 kg·(hm~2·a)~(-1)和2.8 kg·(hm~2·a)~(-1),降水中NH_4~+-N和NO-3-N的混合沉降量分别为7.6 kg·(hm~2·a)~(-1)和6.2 kg·(hm~2·a)~(-1).还原态氮(NH_3和NH_4~+-N)在氮沉降中占主导地位.大气氮素总沉降(干沉降加混合沉降)量为25.6 kg·(hm~2·a)~(-1),为城郊农田提供重要的环境养分;但这一氮素输入量超过了陆地生态系统氮沉降临界负荷[10~20 kg·(hm~2·a)~(-1)],意味着研究区周边林地(如北山)和水体生态系统面临"氮饱和"的环境风险.
This study conducted a full two-year(2014 and 2015) measurements of dry and bulk deposition of atmospheric inorganic nitrogen(N) at the suburb of Xining city,Qinghai province.Dry N deposition fluxes were calculated by multiplying the atmospheric concentrations of NH_3 and NO_2measured using passive samplers with the modeled dry deposition velocities provided by the GEOS-Chem global chemical transport model,while bulk N deposition fluxes were measured using precipitation gauge.Annual mean concentrations of gaseous NH_3 and NO_2averaged 8.8 and 19.6 μg·m-3,respectively,with significantly higher values in 2015 than in 2014.Seasonal mean NH_3 concentrations were higher in spring and summer than in autumn and winter,but the concentrations of NO_2 changed little from season to season,with a small peak in autumn.Annual mean concentrations of NH_4~+-N and NO_3~--N in precipitation averaged 2.2and 1.8 mg·L~(-1),respectively.Concentrations of NH_4~+-N in autumn were ~ 55% lower than those in other seasons,whereas those of NO_3~--N in autumn or winter were ~ 26% higher than those in spring and summer.Dry deposition of NH_3 and NO_2was 9.0 and 2.8kg·(hm~2·a)~(-1),respectively.Bulk deposition of NH_4~+-N and NO_3~--N in precipitation was 7.6 and 6.2 kg·(hm~2·a)~(-1),respectively.Reduced N(gaseous NH_3 and NH_4~+-N in precipitation) was the dominant form of N deposition.The total dry and wet N deposition was25.6 kg·(hm~2·a)~(-1),which represented significant nutrient input from the environment to the suburban farmland,but this amount of deposited N exceeded the critical loads [10-20 kg·(hm~2·a)~(-1)]of terrestrial ecosystems,suggesting a risk of"N saturation"in the local natural environment.
This study conducted a full two-year(2014 and 2015) measurements of dry and bulk deposition of atmospheric inorganic nitrogen(N) at the suburb of Xining city,Qinghai province.Dry N deposition fluxes were calculated by multiplying the atmospheric concentrations of NH_3 and NO_2measured using passive samplers with the modeled dry deposition velocities provided by the GEOS-Chem global chemical transport model,while bulk N deposition fluxes were measured using precipitation gauge.Annual mean concentrations of gaseous NH_3 and NO_2averaged 8.8 and 19.6 μg·m-3,respectively,with significantly higher values in 2015 than in 2014.Seasonal mean NH_3 concentrations were higher in spring and summer than in autumn and winter,but the concentrations of NO_2 changed little from season to season,with a small peak in autumn.Annual mean concentrations of NH_4~+-N and NO_3~--N in precipitation averaged 2.2and 1.8 mg·L~(-1),respectively.Concentrations of NH_4~+-N in autumn were ~ 55% lower than those in other seasons,whereas those of NO_3~--N in autumn or winter were ~ 26% higher than those in spring and summer.Dry deposition of NH_3 and NO_2was 9.0 and 2.8kg·(hm~2·a)~(-1),respectively.Bulk deposition of NH_4~+-N and NO_3~--N in precipitation was 7.6 and 6.2 kg·(hm~2·a)~(-1),respectively.Reduced N(gaseous NH_3 and NH_4~+-N in precipitation) was the dominant form of N deposition.The total dry and wet N deposition was25.6 kg·(hm~2·a)~(-1),which represented significant nutrient input from the environment to the suburban farmland,but this amount of deposited N exceeded the critical loads [10-20 kg·(hm~2·a)~(-1)]of terrestrial ecosystems,suggesting a risk of"N saturation"in the local natural environment.
引文
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[15]Chen D,Wang Y,Mc Elroy M B,et al.Regional CO pollution and export in China simulated by high-resolution nested-grid GEOS-Chem model[J].Atmospheric Chemistry and Physics,2009,9(11):3825-3839.
[16]Zhao Y H,Zhang L,Pan Y P,et al.Atmospheric nitrogen deposition to the northwestern Pacific:seasonal variation and source attribution[J].Atmospheric Chemistry and Physics,2015,15(18):10905-10924.
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[20]Kang Y N,Liu M X,Song Y,et al.High-resolution ammonia emissions inventories in China from 1980 to 2012[J].Atmospheric Chemistry and Physics,2016,16(4):2043-2058.
[21]Warner J X,Wei Z G,Strow L L,et al.The global tropospheric ammonia distribution as seen in the 13-year AIRS measurement record[J].Atmospheric Chemistry and Physics,2016,16(8):5467-5479.
[22]Xu W,Wu Q H,Liu X J,et al.Characteristics of ammonia,acid gases,and PM2.5for three typical land-use types in the North China Plain[J].Environmental Science and Pollution Research,2016,23(2):1158-1172.
[23]Xu W,Zheng K,Liu X J,et al.Atmospheric NH3dynamics at a typical pig farm in China and their implications[J].Atmospheric Pollution Research,2014,5(3):455-463.
[24]Reche C,Viana M,Pandolfi M,et al.Urban NH3levels and sources in a Mediterranean environment[J].Atmospheric Environment,2012,57:153-164.
[25]Streets D G,Bond T C,Carmichael G R,et al.An inventory of gaseous and primary aerosol emissions in Asia in the year 2000[J].Journal of Geophysical Research,2013,108(D21):GTE30-1.
[26]Xu W,Luo X S,Pan Y P,et al.Quantifying atmospheric nitrogen deposition through a nationwide monitoring network across China[J].Atmospheric Chemistry and Physics,2015,15(21):12345-12360.
[27]Yang R,Hayashi K,Zhu B,et al.Atmospheric NH3and NO2concentration and nitrogen deposition in an agricultural catchment of Eastern China[J].Science of the Total Environment,2010,408(20):4624-4632.
[28]Liang T,Tong Y A,Liu X J,et al.High nitrogen deposition in an agricultural ecosystem of Shaanxi,China[J].Environmental Science and Pollution Research,2016,23(13):13210-13221.
[29]Li K H,Liu X J,Song W,et al.Atmospheric nitrogen deposition at two sites in an arid environment of central Asia[J].PLo S One,2013,8(6):e67018.
[30]Kuang F H,Liu X J,Zhu B,et al.Wet and dry nitrogen deposition in the central Sichuan Basin of China[J].Atmospheric Environment,2016,143:39-50.
[31]Cape J N,van der Eerden L J,Sheppard L J,et al.Evidence for changing the critical level for ammonia[J].Environmental Pollution,2009,157(3):1033-1037.
[32]Pan Y P,Tian S L,Liu D W,et al.Fossil fuel combustionrelated emissions dominate atmospheric ammonia sources during severe haze episodes:evidence from15N-stable isotope in sizeresolved aerosol ammonium[J].Environmental Science&Technology,2016,50(15):8049-8056.
[33]Pan Y P,Wang Y S,Tang G Q,et al.Wet and dry deposition of atmospheric nitrogen at ten sites in Northern China[J].Atmospheric Chemistry and Physics,2012,12(14):6515-6535.
[34]Jia Y L,Yu G R,He N P,et al.Spatial and decadal variations in inorganic nitrogen wet deposition in China induced by human activity[J].Scientific Reports,2014,4:3763.
[35]Zhu J X,He N P,Wang Q F,et al.The composition,spatial patterns,and influencing factors of atmospheric wet nitrogen deposition in Chinese terrestrial ecosystems[J].Science of the Total Environment,2015,511:777-785.
[36]Liu L,Zhang X Y,Wang S Q,et al.A review of spatial variation of inorganic nitrogen(N)wet deposition in China[J].PLo S One,2016,11(1):e0146051.
[37]Liu X J,Ju X T,Zhang Y,et al.Nitrogen deposition in agroecosystems in the Beijing area[J].Agriculture,Ecosystems&Environment,2006,113(1-4):370-377.
[38]张菊,康荣华,赵斌,等.内蒙古温带草原氮沉降的观测研究[J].环境科学,2013,34(9):3552-3556.Zhang J,Kang R H,Zhao B,et al.Monitoring nitrogen deposition on temperate grassland in Inner Mongolia[J].Environmental Science,2013,34(9):3552-3556.
[39]Sutton M A,Burkhardt J K,Guerin D,et al.Development of resistance models to describe measurements of bi-directional ammonia surface-atmosphere exchange[J].Atmospheric Environment,1998,32(3):473-480.
[40]Loubet B,Milford C,Hill P W,et al.Seasonal variability of apoplastic NH+4and p H in an intensively managed grassland[J].Plant and Soil,2002,238(1):97-110.
[41]UNECE.Manual on methodologies and criteria for modeling and mapping critical loads and levels and air pollution effects,risks and trends[R/OL].2004.Retrieved from http://www.icpmapping.org.
[2]Galloway J N,Dentener F J,Capone D G,et al.Nitrogen cycles:past,present,and future[J].Biogeochemistry,2004,70(2):153-226.
[3]Vitousek P M,Aber J D,Howarth R W,et al.Human alteration of the global nitrogen cycle:sources and consequences[J].Ecological Applications,1997,7(3):737-750.
[4]Liu X J,Zhang Y,Han W X,et al.Enhanced nitrogen deposition over China[J].Nature,2013,494(7438):459-462.
[5]Ohara T,Akimoto H,Kurokawa J,et al.An Asian emission inventory of anthropogenic emission sources for the period 1980-2020[J].Atmospheric Chemistry and Physics,2007,7(16):4419-4444.
[6]Liu X J,Song L,He C E,et al.Nitrogen deposition as an important nutrient from the environment and its impact on ecosystems in China[J].Journal of Arid Land,2010,2(2):137-143.
[7]张镱锂,李炳元,郑度.论青藏高原范围与面积[J].地理研究,2002,21(1):1-8.Zhang Y L,Li B Y,Zheng D.A discussion on the boundary and area of the Tibetan Plateau in China[J].Geographical Research,2002,21(1):1-8.
[8]Liu Y W,Xu R,Xu X L,et al.Plant and soil responses of an alpine steppe on the Tibetan Plateau to multi-level nitrogen addition[J].Plant and Soil,2013,373(1-2):515-529.
[9]Xu X L,Wanek W,Zhou C P,et al.Nutrient limitation of alpine plants:implications from leaf N:P stoichiometry and leafδ15N[J].Journal of Plant Nutrition and Soil Science,2014,177(3):378-387.
[10]Ma Z,Ma M J,Baskin J M,et al.Responses of alpine meadow seed bank and vegetation to nine consecutive years of soil fertilization[J].Ecological Engineering,2014,70:92-101.
[11]Zheng W,Yao T D,Joswiak D R,et al.Major ions composition records from a shallow ice core on Mt.Tanggula in the central Qinghai-Tibetan Plateau[J].Atmospheric Research,2010,97(1-2):70-79.
[12]Liu Y W,Ri X,Wang Y S,et al.Wet deposition of atmospheric inorganic nitrogen at five remote sites in the Tibetan Plateau[J].Atmospheric Chemistry and Physics,2015,15(20):11683-11700.
[13]Puchalski M A,Sather M E,Walker J T,et al.Passive ammonia monitoring in the United States:comparing three different sampling devices[J].Journal of Environmental Monitoring,2011,13(11):3156-3167.
[14]Shen J L,Li Y,Liu X J,et al.Atmospheric dry and wet nitrogen deposition on three contrasting land use types of an agricultural catchment in subtropical central China[J].Atmospheric Environment,2013,67:415-424.
[15]Chen D,Wang Y,Mc Elroy M B,et al.Regional CO pollution and export in China simulated by high-resolution nested-grid GEOS-Chem model[J].Atmospheric Chemistry and Physics,2009,9(11):3825-3839.
[16]Zhao Y H,Zhang L,Pan Y P,et al.Atmospheric nitrogen deposition to the northwestern Pacific:seasonal variation and source attribution[J].Atmospheric Chemistry and Physics,2015,15(18):10905-10924.
[17]Zhang L,Jacob D J,Knipping E M,et al.Nitrogen deposition to the United States:distribution,sources,and processes[J].Atmospheric Chemistry and Physics,2012,12(10):4539-4554.
[18]Wesely M L.Parameterization of surface resistances to gaseous dry deposition in regional-scale numerical models[J].Atmospheric Environment,1989,23(6):1293-1304.
[19]Clarisse L,Clerbaux C,Dentener F,et al.Global ammonia distribution derived from infrared satellite observations[J].Nature Geoscience,2009,2(7):479-483.
[20]Kang Y N,Liu M X,Song Y,et al.High-resolution ammonia emissions inventories in China from 1980 to 2012[J].Atmospheric Chemistry and Physics,2016,16(4):2043-2058.
[21]Warner J X,Wei Z G,Strow L L,et al.The global tropospheric ammonia distribution as seen in the 13-year AIRS measurement record[J].Atmospheric Chemistry and Physics,2016,16(8):5467-5479.
[22]Xu W,Wu Q H,Liu X J,et al.Characteristics of ammonia,acid gases,and PM2.5for three typical land-use types in the North China Plain[J].Environmental Science and Pollution Research,2016,23(2):1158-1172.
[23]Xu W,Zheng K,Liu X J,et al.Atmospheric NH3dynamics at a typical pig farm in China and their implications[J].Atmospheric Pollution Research,2014,5(3):455-463.
[24]Reche C,Viana M,Pandolfi M,et al.Urban NH3levels and sources in a Mediterranean environment[J].Atmospheric Environment,2012,57:153-164.
[25]Streets D G,Bond T C,Carmichael G R,et al.An inventory of gaseous and primary aerosol emissions in Asia in the year 2000[J].Journal of Geophysical Research,2013,108(D21):GTE30-1.
[26]Xu W,Luo X S,Pan Y P,et al.Quantifying atmospheric nitrogen deposition through a nationwide monitoring network across China[J].Atmospheric Chemistry and Physics,2015,15(21):12345-12360.
[27]Yang R,Hayashi K,Zhu B,et al.Atmospheric NH3and NO2concentration and nitrogen deposition in an agricultural catchment of Eastern China[J].Science of the Total Environment,2010,408(20):4624-4632.
[28]Liang T,Tong Y A,Liu X J,et al.High nitrogen deposition in an agricultural ecosystem of Shaanxi,China[J].Environmental Science and Pollution Research,2016,23(13):13210-13221.
[29]Li K H,Liu X J,Song W,et al.Atmospheric nitrogen deposition at two sites in an arid environment of central Asia[J].PLo S One,2013,8(6):e67018.
[30]Kuang F H,Liu X J,Zhu B,et al.Wet and dry nitrogen deposition in the central Sichuan Basin of China[J].Atmospheric Environment,2016,143:39-50.
[31]Cape J N,van der Eerden L J,Sheppard L J,et al.Evidence for changing the critical level for ammonia[J].Environmental Pollution,2009,157(3):1033-1037.
[32]Pan Y P,Tian S L,Liu D W,et al.Fossil fuel combustionrelated emissions dominate atmospheric ammonia sources during severe haze episodes:evidence from15N-stable isotope in sizeresolved aerosol ammonium[J].Environmental Science&Technology,2016,50(15):8049-8056.
[33]Pan Y P,Wang Y S,Tang G Q,et al.Wet and dry deposition of atmospheric nitrogen at ten sites in Northern China[J].Atmospheric Chemistry and Physics,2012,12(14):6515-6535.
[34]Jia Y L,Yu G R,He N P,et al.Spatial and decadal variations in inorganic nitrogen wet deposition in China induced by human activity[J].Scientific Reports,2014,4:3763.
[35]Zhu J X,He N P,Wang Q F,et al.The composition,spatial patterns,and influencing factors of atmospheric wet nitrogen deposition in Chinese terrestrial ecosystems[J].Science of the Total Environment,2015,511:777-785.
[36]Liu L,Zhang X Y,Wang S Q,et al.A review of spatial variation of inorganic nitrogen(N)wet deposition in China[J].PLo S One,2016,11(1):e0146051.
[37]Liu X J,Ju X T,Zhang Y,et al.Nitrogen deposition in agroecosystems in the Beijing area[J].Agriculture,Ecosystems&Environment,2006,113(1-4):370-377.
[38]张菊,康荣华,赵斌,等.内蒙古温带草原氮沉降的观测研究[J].环境科学,2013,34(9):3552-3556.Zhang J,Kang R H,Zhao B,et al.Monitoring nitrogen deposition on temperate grassland in Inner Mongolia[J].Environmental Science,2013,34(9):3552-3556.
[39]Sutton M A,Burkhardt J K,Guerin D,et al.Development of resistance models to describe measurements of bi-directional ammonia surface-atmosphere exchange[J].Atmospheric Environment,1998,32(3):473-480.
[40]Loubet B,Milford C,Hill P W,et al.Seasonal variability of apoplastic NH+4and p H in an intensively managed grassland[J].Plant and Soil,2002,238(1):97-110.
[41]UNECE.Manual on methodologies and criteria for modeling and mapping critical loads and levels and air pollution effects,risks and trends[R/OL].2004.Retrieved from http://www.icpmapping.org.