民用燃煤排放分级颗粒物中碳组分排放因子
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摘要
中国是全球碳质气溶胶最重要的贡献者之一,民用燃煤排放占有很大的比重.排放因子的不确定性直接影响碳气溶胶排放清单的准确性.本研究基于室内模拟燃烧实验和稀释通道采样系统,采用FA-3型9级撞击采样器采集了3种蜂窝煤(考虑明烧和闷烧)和包括烟煤与褐煤在内的4种块煤燃烧排放的九级粒径颗粒物,采用热光法分析了不同粒径颗粒物中有机碳(OC)和元素碳(EC)的含量,计算得到排放因子.结果表明:(1)对于蜂窝煤的明烧与闷烧,PM2.1中OC排放因子分别为0.07g·kg~(-1)和0.10 g·kg~(-1),EC的排放因子为0.002 g·kg~(-1)和0.001 g·kg~(-1);闷烧排放的有机碳颗粒物高于明烧;元素碳排放因子低于明烧.块煤排放PM2.1中OC与EC排放因子分别是1.4 g·kg~(-1)和0.02 g·kg~(-1),高出蜂窝煤排放一个数量级.(2)粒径分析结果表明,民用煤燃烧排放的颗粒物及其载带的碳组分集中在细颗粒物上,碳组分的质量中值粒径均小于2.5μm,总碳(OC+EC)的排放因子粒径分布表明蜂窝煤燃烧排放的碳组分富集于≤0.43μm粒径段,块煤富集于0.43~0.65μm粒径段.
China is one of the most important contributors to the global burden of carbonaceous aerosols,of which domestic coal combustion occupies a large fraction. Uncertainty in the emission factors( EFs) directly influences the accuracy of corresponding emission inventories. In the present study,based on domestic burning tests with a dilution sampling system,nine size-segregated particle classes emitted from the burning of three kinds of honeycomb coals( under flaming and smoldering burning conditions) and four kinds of chunk coals,including bituminous and lignite,were collected via a cascade impactor( FA-3). Organic and elemental carbon( OC and EC,respectively) were analyzed using the thermal-optical method. The EFs of particulate matter( PM),OC,and EC for nine size ranges were obtained. For honeycomb coals,the EFs of OC and EC in PM2. 1 were 0. 07 g·kg~(-1) and 0. 002 g·kg~(-1),respectively,under flaming burning conditions and 0. 10 g·kg~(-1) and 0. 001 g·kg~(-1),respectively,under smoldering burning conditions. Carbonaceous particles exhibited higher EFs under flaming burning conditions. For chunk coals,the EFs of OC and EC in PM2. 1 were 1. 4 g·kg~(-1) and 0. 02 g·kg~(-1),respectively,which are about one magnitude higher than those for honeycomb coal burning.Particulate matter and its associated carbonaceous components preferred to concentrate in fine particles. The EFs of carbonaceous components peaked at the size of ≤0. 43 μm and 0. 43-0. 65 μm for honeycomb coal burning and chunk coal burning,respectively.
China is one of the most important contributors to the global burden of carbonaceous aerosols,of which domestic coal combustion occupies a large fraction. Uncertainty in the emission factors( EFs) directly influences the accuracy of corresponding emission inventories. In the present study,based on domestic burning tests with a dilution sampling system,nine size-segregated particle classes emitted from the burning of three kinds of honeycomb coals( under flaming and smoldering burning conditions) and four kinds of chunk coals,including bituminous and lignite,were collected via a cascade impactor( FA-3). Organic and elemental carbon( OC and EC,respectively) were analyzed using the thermal-optical method. The EFs of particulate matter( PM),OC,and EC for nine size ranges were obtained. For honeycomb coals,the EFs of OC and EC in PM2. 1 were 0. 07 g·kg~(-1) and 0. 002 g·kg~(-1),respectively,under flaming burning conditions and 0. 10 g·kg~(-1) and 0. 001 g·kg~(-1),respectively,under smoldering burning conditions. Carbonaceous particles exhibited higher EFs under flaming burning conditions. For chunk coals,the EFs of OC and EC in PM2. 1 were 1. 4 g·kg~(-1) and 0. 02 g·kg~(-1),respectively,which are about one magnitude higher than those for honeycomb coal burning.Particulate matter and its associated carbonaceous components preferred to concentrate in fine particles. The EFs of carbonaceous components peaked at the size of ≤0. 43 μm and 0. 43-0. 65 μm for honeycomb coal burning and chunk coal burning,respectively.
引文
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[5]Rasch P J,Collins W D,Eaton B E.Understanding the Indian Ocean Experiment(INDOEX)aerosol distributions with an aerosol assimilation[J].Journal of Geophysical Research:Atmospheres,2001,106(D7):7337-7355.
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[7]Ramanathan V,Ramana M V,Roberts G,et al.Warming trends in Asia amplified by brown cloud solar absorption[J].Nature,2007,448(7153):575-578.
[8]Jones G S,Christidis N,Stott P A.Detecting the influence of fossil fuel and bio-fuel black carbon aerosols on near surface temperature changes[J].Atmospheric Chemistry and Physics,2011,11(2):799-816.
[9]Spracklen D V,Carslaw K S,P?schl U,et al.Global cloud condensation nuclei influenced by carbonaceous combustion aerosol[J].Atmospheric Chemistry and Physics,2011,11(17):9067-9087.
[10]Meehl G A,Arblaster J M,Collins W D.Effects of black carbon aerosols on the Indian monsoon[J].Journal of Climate,2008,21(12):2869-2882.
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[12]Ramanathan V,Carmichael G.Global and regional climate changes due to black carbon[J].Nature Geoscience,2008,1(4):221-227.
[13]Menon S,Hansen J,Nazarenko L,et al.Climate effects of black carbon aerosols in China and India[J].Science,2002,297(5590):2250-2253.
[14]Ming J,Cachier H,Xiao C,et al.Black carbon record based on a shallow Himalayan ice core and its climatic implications[J].Atmospheric Chemistry and Physics,2008,8(5):1343-1352.
[15]Ming J,Xiao C D,Cachier H,et al.Black carbon(BC)in the snow of glaciers in west China and its potential effects on albedos[J].Atmospheric Research,2009,92(1):114-123.
[16]Xu B Q,Cao J J,Hansen J,et al.Black soot and the survival of Tibetan glaciers[J].Proceedings of the National Academy of Sciences of the United States of America,2009,106(52):22114-22118.
[17]Hansen J,Nazarenko L.Soot climate forcing via snow and ice albedos[J].Proceedings of the National Academy of Sciences of the United States of America,2004,101(2):423-428.
[18]Yasunari T J,Bonasoni P,Laj P,et al.Estimated impact of black carbon deposition during pre-monsoon season from Nepal Climate Observatory-Pyramid data and snow albedo changes over Himalayan glaciers[J].Atmospheric Chemistry and Physics,2010,10(14):6603-6615.
[19]Andreae M O.The dark side of aerosols[J].Nature,2001,409(6821):671-672.
[20]Chameides W L,Bergin M.Soot takes center stage[J].Science,2002,297(5590):2214-2215.
[21]Hansen J E,Sato M.Trends of measured climate forcing agents[J].Proceedings of the National Academy of Sciences of the United States of America,2001,98(26):14778-14783.
[22]Hansen J,Sato M,Ruedy R,et al.Global warming in the twenty-first century:an alternative scenario[J].Proceedings of the National Academy of Sciences of the United States of America,2000,97(18):9875-9880.
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[24]Jacobson M Z.Control of fossil-fuel particulate black carbon and organic matter,possibly the most effective method of slowing global warming[J].Journal of Geophysical Research:Atmospheres,2002,107(D19):4410.
[25]Penner J E,Hegg D,Leaitch R.Peer reviewed:unraveling the role of aerosols in climate change[J].Environmental Science&Technology,2001,35(15):332A-340A.
[26]Streets D G,Aunan K.The importance of China's household sector for black carbon emissions[J].Geophysical Research Letters,2005,32(12):L12708.
[27]Künzli N,Kaiser R,Medina S,et al.Public-health impact of outdoor and traffic-related air pollution:a European assessment[J].The Lancet,2000,356(9232):795-801.
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[29]Durant J L,Lafleur A L,Busby Jr W F,et al.Mutagenicity of C24H14PAH in human cells expressing CYP1A1[J].Mutation Research/Genetic Toxicology and Environmental Mutagenesis,1999,446(1):1-14.
[30]中华人民共和国国家统计局.中国统计年鉴2016[M].北京:中国统计出版社,2016.National Bureau of Statistics of the People's Republic of China.China Statistical Yearbook 2016[M].Beijing:China Statistics Press,2016.
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[32]Bond T C,Streets D G,Yarber K F,et al.A technology-based global inventory of black and organic carbon emissions from combustion[J].Journal of Geophysical Research:Atmospheres,2004,109(D14):D14203.
[33]Bond T C,Doherty S J,Fahey D W,et al.Bounding the role of black carbon in the climate system:a scientific assessment[J].Journal of Geophysical Research:Atmospheres,2013,118(11):5380-5552.
[34]Cooke W F,Liousse C,Cachier H,et al.Construction of a 1°×1°fossil fuel emission data set for carbonaceous aerosol and implementation and radiative impact in the ECHAM4 model[J].Journal of Geophysical Research:Atmospheres,1999,104(D18):22137-22162.
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[36]Liousse C,Penner J E,Chuang C,et al.A global threedimensional model study of carbonaceous aerosols[J].Journal of Geophysical Research:Atmospheres,1996,101(D14):19411-19432.
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[38]Streets D G,Gupta S,Waldhoff S T,et al.Black carbon emissions in China[J].Atmospheric Environment,2001,35(25):4281-4296.
[39]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:Atmospheres,2003,108(D21):8809.
[40]Wang R,Tao S,Wang W T,et al.Black carbon emissions in China from 1949 to 2050[J].Environmental Science&Technology,2012,46(14):7595-7603.
[41]Chen Y J,Sheng G Y,Bi X H,et al.Emission factors for carbonaceous particles and polycyclic aromatic hydrocarbons from residential coal combustion in China[J].Environmental Science&Technology,2005,39(6):1861-1867.
[42]Chen Y J,Zhi G R,Feng Y L,et al.Measurements of emission factors for primary carbonaceous particles from residential rawcoal combustion in China[J].Geophysical Research Letters,2006,33(20):L20815.
[43]Zhi G R,Chen Y J,Feng Y L,et al.Emission characteristics of carbonaceous particles from various residential coal-stoves in China[J].Environmental Science&Technology,2008,42(9):3310-3315.
[44]孔少飞,白志鹏,陆炳.民用燃料燃烧排放PM2.5和PM10中碳组分排放因子对比[J].中国环境科学,2014,34(11):2749-2756.Kong S F,Bai Z P,Lu B.Comparative analysis on emission factors of carbonaceous components in PM2.5and PM10from domestic fuels combustion[J].China Environmental Science,2014,34(11):2749-2756.
[45]Shen G F,Xue M,Wei S Y,et al.Influence of fuel moisture,charge size,feeding rate and air ventilation conditions on the emissions of PM,OC,EC,parent PAHs,and their derivatives from residential wood combustion[J].Journal of Environmental Sciences,2013,25(9):1808-1816.
[46]Shen G F,Xue M,Wei S Y,et al.Influence of fuel mass load,oxygen supply and burning rate on emission factor and size distribution of carbonaceous particulate matter from indoor corn straw burning[J].Journal of Environmental Sciences,2013,25(3):511-519.
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