广州大气颗粒物水溶性有机氮的粒径分布特征和来源分析
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摘要
水溶性有机氮(WSON)在大气化学和气候变化中具有重要作用,目前鲜有针对WSON粒径分布的研究。本研究利用大流量采样器在2014年9月至2015年7月期间采集了广州市各个季节PM_(10)中不同粒径段(<0.49μm、0.49～0.95μm、0.95～1.5μm、1.5～3.0μm、3.0～7.2μm、7.2～10μm)大气颗粒物样品共100个,分析了其中的水溶性总氮(WSTN)、WSON以及水溶性无机氮(WSIN)含量。结果表明,各个粒径段中WSON的浓度呈现相似的季节变化特征,秋、冬季较高,春、夏季较低。WSON主要分布在细颗粒物上,PM_3中WSON的季节平均浓度在1.15～2.62μg/m~3范围内,占PM_(10)中WSON总量的63%～71%。WSON的粒径分布呈现单峰分布,主要富集在0.49～1.5μm粒径段。主成分分析/绝对主成分得分(PCA/APCS)分析表明,<0.49μm颗粒物上的WSON主要来源于本地化石燃料的燃烧排放;0.49～0.95μm颗粒物的WSON主要来源于建筑扬尘和光化学氧化二次生成过程;0.95～1.5μm颗粒物的WSON主要来源于光化学氧化二次生成过程。研究结果增加了目前对于WSON粒径分布特征和来源的认识。
Water-soluble organic nitrogen(WSON)plays an important role in atmospheric chemistry and climatic change.However,few studies have focused on WSON in size-segregated particles.In this study,size-segregated particle samples in the size ranges of<0.49μm,0.49–0.95μm,0.95–1.5μm,1.5–3.0μm,3.0–7.2μm,7.2–10μm were collected in Guangzhou,China from September 2014 to July 2015 by a high-volume sampler.Samples were analyzed for water-soluble total nitrogen(WSTN),WSON and and water-soluble inorganic ions(WSIN).The concentrations of WSON in each size range showed a similar seasonal trend with higher concentrations in autumn and winter and lower concentrations in spring and summer.The seasonal average concentrations of WSON in PM_3 ranged from 1.15 to 2.62μg/m~3,contributing to 63%–71%of the WSON in PM_(10).The concentrations of WSON in particles<3μm exhibited a unimodal distribution in four seasons,enriching in the 0.49–0.95μm particles.The principal component analysis(PCA)/absolute principal component scores(APCS)analysis showed that WSON can be mainly attributed to the burning of local fossil fuels in particles<0.49μm,to construction dust and photochemical oxidation leading to its secondary formation in 0.49–0.95μm particles;and to photochemical oxidation leading to secondary formation alone in 0.95–1.5μm particles.Our research improves our understanding of the environmental geochemical processes of organic nitrogen compounds.
Water-soluble organic nitrogen(WSON)plays an important role in atmospheric chemistry and climatic change.However,few studies have focused on WSON in size-segregated particles.In this study,size-segregated particle samples in the size ranges of<0.49μm,0.49–0.95μm,0.95–1.5μm,1.5–3.0μm,3.0–7.2μm,7.2–10μm were collected in Guangzhou,China from September 2014 to July 2015 by a high-volume sampler.Samples were analyzed for water-soluble total nitrogen(WSTN),WSON and and water-soluble inorganic ions(WSIN).The concentrations of WSON in each size range showed a similar seasonal trend with higher concentrations in autumn and winter and lower concentrations in spring and summer.The seasonal average concentrations of WSON in PM_3 ranged from 1.15 to 2.62μg/m~3,contributing to 63%–71%of the WSON in PM_(10).The concentrations of WSON in particles<3μm exhibited a unimodal distribution in four seasons,enriching in the 0.49–0.95μm particles.The principal component analysis(PCA)/absolute principal component scores(APCS)analysis showed that WSON can be mainly attributed to the burning of local fossil fuels in particles<0.49μm,to construction dust and photochemical oxidation leading to its secondary formation in 0.49–0.95μm particles;and to photochemical oxidation leading to secondary formation alone in 0.95–1.5μm particles.Our research improves our understanding of the environmental geochemical processes of organic nitrogen compounds.
引文
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[2]Murphy S M,Sorooshian A,Kroll J H,Ng N L,Chhabra P,Tong C,Surratt J D,Knipping E,Flagan R C,Seinfeld J H.Secondary aerosol formation from atmospheric reactions of aliphatic amines[J].Atmos Chem Phys,2007,7(9):2313-2337.
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[4]Ho K F,Ho S S H,Huang R J,Liu S X,Cao J J,Zhang T,Chuang H C,Chan C S,Hu D,Tian L W.Characteristics of water-soluble organic nitrogen in fine particulate matter in the continental area of China[J].Atmos Environ,2015,106:252-261.
[5]Cornell S,Mace K,Coeppicus S,Duce R,Huebert B,Jickells T,Zhuang L Z.Organic nitrogen in Hawaiian rain and aerosol[J].J Geophys Res Atmos,2001,106(D8):7973-7983.
[6]Zhang Q,Anastasio C.Free and combined amino compounds in atmospheric fine particles(PM2.5)and fog waters from Northern California[J].Atmos Environ,2003,37(16):2247-2258.
[7]Landvik N E,Gorria M,Arlt V M,Asare N,Solhaug A,Lagadic-Gossmann D,Holme J A.Effects of nitrated-polycyclic aromatic hydrocarbons and diesel exhaust particle extracts on cell signalling related to apoptosis:Possible implications for their mutagenic and carcinogenic effects[J].Toxicology,2007,231(2/3):159-174.
[8]Luo P,Ni H G,Bao L J,Li S M,Zeng E Y.Size distribution of airborne particle-bound polybrominated diphenyl ethers and its implications for dry and wet deposition[J].Environ Sci Technol,2014,48(23):13793-13799.
[9]Zhang Q,Anastasio C.Chemistry of fog waters in California’s Central Valley-Part 3:Concentrations and speciation of organic and inorganic nitrogen[J].Atmos Environ,2001,35(32):5629-5643.
[10]Nakamura T,Ogawa H,Maripi D K,Uematsu M.Contribution of water soluble organic nitrogen to total nitrogen in marine aerosols over the East China Sea and western North Pacific[J].Atmos Environ,2006,40(37):7259-7264.
[11]Rastogi N,Zhang X L,Edgerton E S,Ingall E,Weber R J.Filterable water-soluble organic nitrogen in fine particles over the southeastern USA during summer[J].Atmos Environ,2011,45(33):6040-6047.
[12]Facchini M C,Decesari S,Rinaldi M,Carbone C,Finessi E,Mircea M,Fuzzi S,Moretti F,Tagliavini E,Ceburnis D,O'Dowd C D.Important source of marine secondary organic aerosol from biogenic amines[J].Environ Sci Technol,2008,42(24):9116-9121.
[13]Violaki K,Mihalopoulos N.Water-soluble organic nitrogen(WSON)in size-segregated atmospheric particles over the Eastern Mediterranean[J].Atmos Environ,2010,44(35):4339-4345.
[14]Duan F,Liu X,He K,Dong S.Measurements and characteristics of nitrogen-containing compounds in atmospheric particulate matter in Beijing,China[J].Bull Environ Contam Toxicol,2009,82:332-337.
[15]石金辉,韩静,范得国,祁建华,高会旺.青岛大气气溶胶中水溶性有机氮对总氮的贡献[J].环境科学,2011,32(1):1-8.Shi Jin-hui,Han Jing,Fan De-guo,Qi Jian-hua,Gao Huiwang.Contribution of water soluble organic nitrogen to total nitrogen in atmospheric aerosols in Qingdao[J].Environ Sci,2011,32(1):1-8(in Chinese with English abstract).
[16]程玉婷,王格慧,孙涛,成春雷,孟静静,任艳芹,李建军.西安冬季非灰霾天与灰霾天PM2.5中水溶性有机氮污染特征比较[J].环境科学,2014,35(7):2468-2476.Cheng Yu-ting,Wang Ge-hui,Sun Tao,Cheng Chun-lei,Meng Jing-jing,Ren Yan-qin,Li Jian-jun.Characteristics of water-soluble organic nitrogen of PM2.5 in Xi’an during wintertime non-haze and haze periods[J].Environ Sci,2014,35(7):2468-2476(in Chinese with English abstract).
[17]徐玢花,杜艳,胡俊超,孙文文,冯加良.上海PM2.5中水溶性有机氮的污染特征[J].地球化学,2016,45(2):190-198.Xu Bin-hua,Du Yan,Hu Jun-chao,Sun Wen-wen,Feng Jialiang.Characteristics of water-soluble organic nitrogen in PM2.5 in Shanghai[J].Geochimica,2016,45(2):190-198(in Chinese with English abstract).
[18]Lesworth T,Baker A R,Jickells T.Aerosol organic nitrogen over the remote Atlantic Ocean[J].Atmos Environ,2010,44(15):1887-1893.
[19]Shi J H,Gao H W,Qi J H,Zhang J,Yao X H.Sources,compositions,and distributions of water-soluble organic nitrogen in aerosols over the China Sea[J].J Geophys Res,2010,115(D17303).doi:10.1029/2009JD013238
[20]Zhang Q,Anastasio C,Jimemez-Cruz M.Water-soluble organic nitrogen in atmospheric fine particles(PM2.5)from northern California[J].J Geophys Res Atmos,2002,107(D11):AAC3-1-AAC 3-9.
[21]Mace K A.Water-soluble organic nitrogen in Amazon Basin aerosols during the dry(biomass burning)and wet seasons[J].JGeophys Res Atmos,2003,108(D16).doi:10.1029/2003JD003557
[22]Montero-Martinez G,Rinaldi M,Gilardoni S,Giulianelli L,Paglione M,Decesari S,Fuzzi S,Facchini M C.On the water-soluble organic nitrogen concentration and mass size distribution during the fog season in the Po Valley,Italy[J].Sci Total Environ,2014,485/486:103-109.
[23]Yu X,Yu Q Q,Zhu M,Tang M J,Li S,Yang W Q,Zhang YL,Deng W,Li G H,Yu Y G,Huang Z H,Song W,Ding X,Hu Q H,Li J,Bi X H,Wang X M.Water soluble organic nitrogen(WSON)in ambient fine particles over a megacity in South China:Spatiotemporal variations and source apportionment[J].J Geophys Res Atmos,2017,122(23):13045-13060.
[24]Miyazaki Y,Fu P Q,Ono K,Tachibana E,Kawamura K.Seasonal cycles of water-soluble organic nitrogen aerosols in a deciduous broadleaf forest in northern Japan[J].J Geophys Res Atmos,2014,119(3):1440-1454.
[25]Li J,Fang Y T,Yoh M,Wang X M,Wu Z Y,Kuang Y W,Wen D Z.Organic nitrogen deposition in precipitation in metropolitan Guangzhou city of southern China[J].Atmos Res,2012,113:57-67.
[26]Tao J,Zhang L M,Cao J J,Zhong L J,Chen D S,Yang Y H,Chen D H,Chen L G,Zhang Z S,Wu Y F,Xia Y J,Ye S Q,Zhang R J.Source apportionment of PM2.5 at urban and suburban areas of the Pearl River Delta region,south China-With emphasis on ship emissions[J].Sci Total Environ,2017,574:1559-1570.
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[28]黄欢.广州城区气溶胶中水溶性有机物分布特征及氧化潜能浅析[D].广州:中国科学院广州地球化学研究所,2016.Huang Huan.The characterization of water-soluble organic matter and oxidative potential of atmospheric aerosols at the urban area of Guangzhou[D].Guangzhou:Guangzhou Institute of Geochemistry,Chinese Academy of Sciences,2016(in Chinese with English abstract).
[29]Cheng Z L,Lam K S,Chan L Y,Wang T,Cheng K K.Chemical characteristics of aerosols at coastal station in Hong Kong.I.Seasonal variation of major ions,halogens and mineral dusts between 1995 and 1996[J].Atmos Environ,2000,34(17):2771-2783.
[30]龚识懿.上海大气PM2.5中有机氮污染特征及来源解析[D].上海:上海大学,2013.Gong Shi-yi.The distribution and sources of organic nitrogen in PM2.5 in Shanghai,China[D].Shanghai:Shanghai University,2013(in Chinese with English abstract).
[31]徐玢花.上海PM2.5中水溶性有机氮的浓度特征和来源解析[D].上海:上海大学,2015.Xu Bin-hua.Characteristics and sources of water-soluble organic nitrogen in PM2.5 in Shanghai,China[D].Shanghai:Shanghai University,2015(in Chinese with English abstract).
[32]You Y,Kanawade V P,de Gouw J A,Guenther A B,Madronich S,Sierra-Hernandez M R,Lawler M,Smith J N,Takahama S,Ruggeri G,Koss A,Olson K,Baumann K,Weber R J,Nenes A,Guo H,Edgerton E S,Porcelli L,Brune W H,Goldstein A H,Lee S H.Atmospheric amines and ammonia measured with a chemical ionization mass spectrometer(CIMS)[J].Atmos Chem Phys,2014,14(22):12181-12194.
[33]Miller S L,Anderson M J,Daly E P,Milford J B.Source apportionment of exposures to volatile organic compounds.I.Evaluation of receptor models using simulated exposure data[J].Atmos Environ,2002,36(22):3629-3641.
[34]Guo H,Lee S C,Li W M,Cao J J.Source characterization of BTEX in indoor microenviron-ments in Hong Kong[J].Atmos Environ,2003,37(1):73-82.
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