常州市冬季PM_(2.5)中类腐殖质昼夜特征分析
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摘要
为探讨常州冬季大气气溶胶中类腐殖质(HULIS)的昼夜变化特征,在常州市城郊于2017年1月1日～2月28日采集了64个细颗粒物(PM_(2.5))样品,分析获取了类腐殖碳(HULIS-C)的浓度和光学变化特征.冬季PM_(2.5)昼夜平均质量浓度分别为122. 60μg·m~(-3)和111. 72μg·m~(-3),HULIS-C的昼夜平均质量浓度分别为4. 18μg·m~(-3)和3. 74μg·m~(-3),白天均高于夜晚.紫外光谱分析结果表明,HULIS/WSOA(水溶性有机质)于250 nm处的吸光度比值(昼:77%,夜:75%)明显大于HULIS-C/WSOC(水溶性碳)的浓度比值(昼:51%,夜:50%),表明较多的高紫外吸收物质和多聚共轭芳香结构存在于HULIS中;昼夜HULIS在250 nm和365 nm光下的吸光度比值(E250/E365)和特征紫外吸光度(SUVA280)的差异小,说明HULIS在芳香度和分子量上昼夜差异小,且昼夜HULIS化学性质及组成相近;进一步分析了HULIS的光吸收效率(MAE365)和光吸收指数(AAE300-400),发现昼夜没有明显差异.此外,通过HULIS-C和PM_(2.5)中其他化学组分的相关性分析,定性了解常州市冬季HULIS的主要影响因素,HULIS-C来源上受到了生物质燃烧、化石燃料燃烧、工厂排放以及二次生成的共同影响;而昼夜之间对比表明,昼间HULIS主要受到二次生成的影响,而夜间HULIS来源上除受到白天二次生成影响外,也受到了一次燃烧排放的影响.
To investigate the characteristics of diurnal variation of humic-like substances( HULIS) in atmospheric aerosols during winter in Changzhou,a total of 64 fine particle( PM_(2.5)) samples were collected from January 1 to February 28,2017. In this study,the concentration as well as light absorption parameters of humic-like substances of carbon( HULIS-C) were examined. The results showed that the average day PM_(2.5) and HULIS-C concentrations were 122. 60 μg·m~(-3) and 4. 18 μg·m~(-3),respectively,slightly higher than those( 111. 72 μg·m~(-3) and 3. 74 μg·m~(-3)) at night. Via UV-vis analysis,we found that the ratios of absorbance at 250 nm( A250) of HULIS and WSOA( day: ～ 77%,night: ～ 75%) were significantly higher than the concentration ratios of HULIS-C and WSOC( day: ～ 51%,night: ～ 50%),indicating that more UV-absorbing substances and poly-conjugated aromatic structures exist in HULIS. The daytime E250/E365 and SUVA280 in HULIS were close to the nighttime ones,indicating that there was no obvious difference between day and night in HULIS with reference to aromaticity and molecular weight. There were no significant differences in MAE365 and AAE300-400 of HULIS between day and night. In addition,to obtain the main influencing factors of HULIS in winter in Changzhou,the correlation analysis of HULIS-C and other chemical components were conducted. The results show that biomass burning,fossil fuel combustion,factory emissions,and especially secondary formation,were the main influencing factors. Moreover,daytime HULIS were mainly influenced by secondary reaction of anthropogenic precursor contaminants,while nighttime HULIS were affected not only by secondary formation by but by also primary combustion emissions.
To investigate the characteristics of diurnal variation of humic-like substances( HULIS) in atmospheric aerosols during winter in Changzhou,a total of 64 fine particle( PM_(2.5)) samples were collected from January 1 to February 28,2017. In this study,the concentration as well as light absorption parameters of humic-like substances of carbon( HULIS-C) were examined. The results showed that the average day PM_(2.5) and HULIS-C concentrations were 122. 60 μg·m~(-3) and 4. 18 μg·m~(-3),respectively,slightly higher than those( 111. 72 μg·m~(-3) and 3. 74 μg·m~(-3)) at night. Via UV-vis analysis,we found that the ratios of absorbance at 250 nm( A250) of HULIS and WSOA( day: ～ 77%,night: ～ 75%) were significantly higher than the concentration ratios of HULIS-C and WSOC( day: ～ 51%,night: ～ 50%),indicating that more UV-absorbing substances and poly-conjugated aromatic structures exist in HULIS. The daytime E250/E365 and SUVA280 in HULIS were close to the nighttime ones,indicating that there was no obvious difference between day and night in HULIS with reference to aromaticity and molecular weight. There were no significant differences in MAE365 and AAE300-400 of HULIS between day and night. In addition,to obtain the main influencing factors of HULIS in winter in Changzhou,the correlation analysis of HULIS-C and other chemical components were conducted. The results show that biomass burning,fossil fuel combustion,factory emissions,and especially secondary formation,were the main influencing factors. Moreover,daytime HULIS were mainly influenced by secondary reaction of anthropogenic precursor contaminants,while nighttime HULIS were affected not only by secondary formation by but by also primary combustion emissions.
引文
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[3]陈多宏,李梅,黄渤,等.区域大气细粒子污染特征及快速来源解析[J].中国环境科学,2016,36(3):651-659.Chen D H,Li M,Huang B,et al.The pollution characteristics and source apportionment of regional atmospheric fine particles[J].China Environmental Science,2016,36(3):651-659.
[4]Graber E R,Rudich Y.Atmospheric HULIS:how humic-like are they?A comprehensive and critical review[J].Atmospheric Chemistry and Physics,2006,6(3):729-753.
[5]Fan X J,Li M J,Cao T,et al.Optical properties and oxidative potential of water-and alkaline-soluble brown carbon in smoke particles emitted from laboratory simulated biomass burning[J].Atmospheric Environment,2018,194:48-57.
[6]Gysel M,Weingartner E,Nyeki S,et al.Hygroscopic properties of water-soluble matter and humic-like organics in atmospheric fine aerosol[J].Atmospheric Chemistry and Physics,2004,4(1):35-50.
[7]Facchini M C,Mircea M,Fuzzi S,et al.Cloud albedo enhancement by surface-active organic solutes in growing droplets[J].Nature,1999,401(6750):257-259.
[8]Wang B B,Knopf D A.Heterogeneous ice nucleation on particles composed of humic-like substances impacted by O3[J].Journal of Geophysical Research,2011,116(D3):D03205.
[9]范行军.气溶胶中类腐殖质的分离定量、化学表征和来源分析研究[D].北京:中国科学院研究生院(广州地球化学研究所),2015.Fan X J.Isolation,characterization and source apportionment of Humic-Like Substances in atmospheric aerosols[D].Beijing:Guangzhou Institute of Geochemistry,Chinese Academy of Sciences,2015.
[10]Havers N,Burba P,Lambert J,et al.Spectroscopic Characterization of humic-like substances in airborne particulate matter[J].Journal of Atmospheric Chemistry,1998,29(1):45-54.
[11]Altieri K E,Seitzinger S P,Carlton A G,et al.Oligomers formed through in-cloud methylglyoxal reactions:chemical composition,properties,and mechanisms investigated by ultrahigh resolution FT-ICR mass spectrometry[J].Atmospheric Environment,2008,42(7):1476-1490.
[12]Lin P,Huang X F,He L Y,et al.Abundance and size distribution of HULIS in ambient aerosols at a rural site in South China[J].Journal of Aerosol Science,2010,41(1):74-87.
[13]Lin P,Engling G,Yu J Z.Humic-like substances in fresh emissions of rice straw burning and in ambient aerosols in the Pearl River Delta Region,China[J].Atmospheric Chemistry and Physics,2010,10(14):6487-6500.
[14]Mayol-Bracero O L,Guyon P,Graham B,et al.Water-soluble organic compounds in biomass burning aerosols over Amazonia 2.Apportionment of the chemical composition and importance of the polyacidic fraction[J].Journal of Geophysical Research,2002,107(D20):8091.
[15]Gon9alves C,Alves C,Evtyugina M,et al.Characterisation of PM10emissions from woodstove combustion of common woods grown in Portugal[J].Atmospheric Environment,2010,44(35):4474-4480.
[16]Schmidl C,Bauer H,Dattler A,et al.Chemical characterisation of particle emissions from burning leaves[J].Atmospheric Environment,2008,42(40):9070-9079.
[17]Baduel C,Voisin D,Jaffrezo J L.Seasonal variations of concentrations and optical properties of water soluble HULIScollected in urban environments[J].Atmospheric Chemistry and Physics,2010,10(9):4085-4095.
[18]Kuang B Y,Lin P,Huang X H H,et al.Sources of humic-like substances in the Pearl River Delta,China:positive matrix factorization analysis of PM2.5major components and source markers[J].Atmospheric Chemistry and Physics,2015,15(4):1995-2008.
[19]Lin P,Rincon A G,Kalberer M,et al.Elemental composition of HULIS in the Pearl River Delta Region,China:results inferred from positive and negative electrospray high resolution mass spectrometric data[J].Environmental Science&Technology,2012,46(14):7454-7462.
[20]程玉婷,王格慧,孙涛,等.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 Y T,Wang G H,Sun T,et al.Characteristics of watersoluble organic nitrogen of PM2.5in Xi'an during wintertime nonhaze and haze periods[J].Environmental Science,2014,35(7):2468-2476.
[21]Claeys M,Vermeylen R,Yasmeen F,et al.Chemical characterisation of humic-like substances from urban,rural and tropical biomass burning environments using liquid chromatography with UV/vis photodiode array detection and electrospray ionisation mass spectrometry[J].Environmental Chemistry,2012,9(3):273-284.
[22]徐丽.长三角城市群16城市经济效率及其影响因素研究[D].上海:复旦大学,2010.
[23]常州市统计局,国家统计局常州调查队.常州统计年鉴[M].北京:中国统计出版社,2017.
[24]王昂扬,潘岳,童岩冰.长三角主要城市空气污染时空分布特征研究[J].环境保护科学,2015,41(5):131-136.Wang A Y,Pan Y,Tong Y B.Research of temporal and spatial distribution of air pollution in the major cities of the Yangtze River Delta[J].Environmental Protection Science,2015,41(5):131-136.
[25]李清,黄雯倩,马帅帅,等.常州春季PM2.5中WSOC和WSON的污染特征与来源解析[J].环境科学,2019,40(1):94-103.Li Q,Huang W Q,Ma S S,et al.Characteristics and sources of water-soluble organic carbon/nitrogen in PM2.5during spring in Changzhou[J].Environmental Science,2019,40(1):94-103.
[26]Ye Z L,Li Q,Ma S S,et al.Summertime day-night differences of PM2.5components(Inorganic Ions,OC,EC,WSOC,WSON,HULIS,and PAHs)in Changzhou,China[J].Atmosphere,2017,8(10):189.
[27]张伟,姬亚芹,李金,等.鞍山市夏冬季PM2.5中碳组分化学特征及来源解析[J].中国环境科学,2017,37(5):1657-1662.Zhang W,Ji Y Q,Li J,et al.The characteristics and source apportionment of carbon fractions in PM2.5during summer-winter period in Anshan City[J].China Environmental Science,2017,37(5):1657-1662.
[28]Feczko T,Puxbaum H,Kasper-Giebl A,et al.Determination of water and alkaline extractable atmospheric humic-l ike substances with the TU Vienna HULIS analyzer in samples from six background sites in Europe[J].Journal of Geophysical Research,2007,112(D23):D23S10.
[29]Kiss G,Varga B,Galambos I,et al.Characterization of watersoluble organic matter isolated from atmospheric fine aerosol[J].Journal of Geophysical Research,2002,107(D21):ICC 1-1-ICC 1-8.
[30]Song J Z,He L L,Peng P A,et al.Chemical and isotopic composition of humic-like substances(HULIS)in ambient aerosols in Guangzhou,South China[J].Aerosol Science and Technology,2012,46(5):533-546.
[31]黄众思,修光利,蔡婧,等.大气PM2.5中水溶性有机碳和类腐殖质碳的季节变化特征[J].环境科学学报,2013,33(10):2664-2670.Huang Z S,Xiu G L,Cai J,et al.Seasonal characterization of water-soluble organic carbon and humic-like substance carbon in atmospheric PM2.5[J].Acta Scientiae Circumstantiae,2013,33(10):2664-2670.
[32]倪海燕,韩永明,曹军骥.西安水溶性类腐殖质气溶胶(HULIS)的污染特征及其来源[A].见:十一届全国气溶胶会议暨第十届海峡两岸气溶胶技术研讨会摘要集[C].武汉:中国颗粒学会气溶胶专业委员会,2013.
[33]Tan J H,Xiang P,Zhou X M,et al.Chemical characterization of humic-like substances(HULIS)in PM2.5in Lanzhou,China[J].Science of the Total Environment,2016,573:1481-1490.
[34]Kumar V,Goel A,Rajput P.Compositional and surface characterization of HULIS by UV-Vis,FTIR,NMR and XPS:Wintertime study in Northern India[J].Atmospheric Environment,2017,164:468-475.
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