春节前后华北平原农村地区黑碳浓度及来源
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摘要
在河南某农村站点利用黑碳仪(AE33)对春节前后(2018年2月12日～3月12日)黑碳气溶胶(eBC)进行在线连续监测,获得其质量浓度、昼夜变化及来源.结果表明:春节期间的eBC浓度最高,(8.22±4.17)μg/m~3,该时期人为活动对eBC影响最为明显.春节前,生物质燃烧产生的eBC占其总浓度百分比最大,为(41.1±5.3)%,并随时间推移逐渐减小,降至(26.8±12.0)%.AAE(1.40±0.16)说明,该地区春节前后eBC的化石燃料排放和生物质燃烧贡献程度接近.与城市点位相比,本研究的AAE值较高.春节前后,观测地区的eBC昼夜变化存在2个明显高值时段,分别在7:00～9:00和20:00左右.春节期间的eBC昼夜变化无明显波动.根据浓度权重轨迹分析显示,春节期间eBC的潜在源区有山西、陕西、安徽和江苏等省份,其他时期集中在河南、湖北境内.本研究对于识别冬季农村燃烧源排放黑碳演化特征及其对区域重霾形成和发展的影响具有重要意义,也可为黑碳气溶胶气候、环境和健康模拟提供基础数据.
To obtain the mass concentrations, diurnal variations and sources of black carbon(eBC) aerosol around the Chinese spring festival(SF) in rural regions of the North China Plain, one-month(2018-2-12～2018-3-12) online continuous measurement of black carbon was conducted at a rural site in Henan province. During the SF, the e BC concentration was highest,(8.22±4.17)μg/m~3, suggesting intensive emissions from anthropogenic activities. Before the SF, the contribution of biomass burning was the largest(41.1±5.3)%, and then gradually decreased down to(26.8±12.0)%. During the study period, the calculated AAE value(1.40±0.16) indicated that the contribution of biomass burning to eBC was close to that of fossil fuel in this area. Compared with some urban sites, the AAE value in this study was higher. Before and after the SF, the eBC mass concentrations show significant diurnal variations, with 2 peak values occurring at 07:00～09:00 and around 20:00(local time). During the SF, the diurnal variation of eBC mass concentration did not fluctuate obviously. According to the concentration-weighted trajectories analysis, the main potential source regions of eBC were Shanxi, Shaanxi, Anhui, and Jiangsu provinces during the SF. In other two periods, Henan and Hubei provinces could be the main impact regions. This study is meaningful to identify the impact of BC emitted from rural combustion sources on regional haze formation and evolution, and it can also supply the dataset for corresponding modeling of BC's impacts on climate, air quality and human health.
To obtain the mass concentrations, diurnal variations and sources of black carbon(eBC) aerosol around the Chinese spring festival(SF) in rural regions of the North China Plain, one-month(2018-2-12～2018-3-12) online continuous measurement of black carbon was conducted at a rural site in Henan province. During the SF, the e BC concentration was highest,(8.22±4.17)μg/m~3, suggesting intensive emissions from anthropogenic activities. Before the SF, the contribution of biomass burning was the largest(41.1±5.3)%, and then gradually decreased down to(26.8±12.0)%. During the study period, the calculated AAE value(1.40±0.16) indicated that the contribution of biomass burning to eBC was close to that of fossil fuel in this area. Compared with some urban sites, the AAE value in this study was higher. Before and after the SF, the eBC mass concentrations show significant diurnal variations, with 2 peak values occurring at 07:00～09:00 and around 20:00(local time). During the SF, the diurnal variation of eBC mass concentration did not fluctuate obviously. According to the concentration-weighted trajectories analysis, the main potential source regions of eBC were Shanxi, Shaanxi, Anhui, and Jiangsu provinces during the SF. In other two periods, Henan and Hubei provinces could be the main impact regions. This study is meaningful to identify the impact of BC emitted from rural combustion sources on regional haze formation and evolution, and it can also supply the dataset for corresponding modeling of BC's impacts on climate, air quality and human health.
引文
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[6] Menon S, Hansen J E, Nazarenko L, et al. Climate effects of black carbon aerosols in China and India[J]. Science, 2002,297(5590):2250-2253.
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[9] Janssen N A H, Hoek G, Simic-Lawson M, et al. Black Carbon as an Additional Indicator of the Adverse Health Effects of Airborne Particles Compared with PM10and PM2.5[J]. Environmental Health Perspectives, 2011,119(12):1691-1699.
[10] Xu Z, Huang X, Nie W, et al. Influence of synoptic condition and holiday effects on VOCs and ozone production in the Yangtze River Delta region, China[J]. Atmospheric Environment, 2017,168:112-124.
[11] Ru-Jin H, Yanlin Z, Carlo B, et al. High secondary aerosol contribution to particulate pollution during haze events in China[J].Nature, 2014,514(7521):218-222.
[12] Chang X, Wang S, Zhao B, et al. Assessment of inter-city transport of particulate matter in the Beijing-Tianjin-Hebei region[J].Atmospheric Chemistry and Physics, 2017:1-28.
[13] Wu S, Deng F, Wei H, et al. Association of cardiopulmonary health effects with source-appointed ambient fine particulate in Beijing,China:a combined analysis from the Healthy Volunteer Natural Relocation(HVNR)study[J]. Environmental Science and Technology,2014,48(6):3438-3448.
[14]李珊珊,程念亮,徐峻,等.2014年京津冀地区PM2.5浓度时空分布及来源模拟[J].中国环境科学, 2015,35(10):2908-2916.Li S S, Cheng N L, XU J. Spatial and temporal distrubions and source simulation of PM2.5 in Beijing-Tianjin-Hebei region in 2014[J].China Environmental Science, 2015,35(10):2908-2916.
[15] Chen H, Wang H. Haze Days in North China and the Associated Atmospheric Circulations Based on Daily Visibility Data from 1960 to2012[J]. Journal of Geophysical Research Atomosphere, 2015,120(12):5895-5909.
[16] Wang W, Simonich S, Giri B, et al. Atmospheric concentrations and air–soil gas exchange of polycyclic aromatic hydrocarbons(PAHs)in remote, rural village and urban areas of Beijing–Tianjin region, North China[J]. Science of The Total Environment, 2011,409(15):2942-2950.
[17] Wang Z, Xin H, Ding A. Dome effect of black carbon and its key influencing factors:A one-dimensional modelling study[J].Atmospheric Chemistry and Physics, 2018,18(4):1-29.
[18] Chen D, Liu X, Lang J, et al. Estimating the contribution of regional transport to PM2.5 air pollution in a rural area on the North China Plain[J]. Science of The Total Environment, 2017,583:280-291.
[19]杨浩,白永清,刘琳,等.基于轨迹聚类河南地区大气污染过程空气输送通道研究[J].气象与环境学报, 2017,33(4):29-39.Yang H, Bai Y Q, Liu L, et al. Analysis of air transport channels during pollution process in He'nan province based on trajector clustering[J]. Journal of Meteorology and Environment, 2017,33(4):29-39.
[20] Feng J, Yu H, Su X, et al. Chemical composition and source apportionment of PM2.5 during Chinese Spring Festival at Xinxiang, a heavily polluted city in North China:Fireworks and health risks[J].Atmospheric Research, 2016,182:176-188.
[21] Ji D, Cui Y, Li L, et al. Characterization and source identification of fine particulate matter in urban Beijing during the 2015 Spring Festival[J]. Science of the Total Environment, 2018,s628–629:430-440.
[22] Zhao S, Chen L, Yan J, et al. Characterization of lead-containing aerosol particles in Xiamen during and after Spring Festival by single-particle aerosol mass spectrometry[J]. Science of the Total Environment, 2017,580:1257-1267.
[23] Tian Y Z, Wang J, Peng X, et al. Estimation of the direct and indirect impacts of fireworks on the physicochemical characteristics of atmospheric PM10 and PM2.5[J]. Atmospheric Chemistry and Physics,2014,14(18):9469-9479.
[24] Kong S F, Li L, Li X X, et al. The impacts of firework burning at the Chinese Spring Festival on air quality:insights of tracers, source evolution and aging processes[J]. Atmospheric Chemistry and Physics,2015,15(4):2167-2184.
[25] Huang K, Zhuang G, Lin Y, et al. Impact of anthropogenic emission on air quality over a megacity–revealed from an intensive atmospheric campaign during the Chinese Spring Festival[J].Atmospheric Chemistry and Physics, 2012,12(23):11631-11645.
[26] Jiang Q, Sun Y L, Wang Z, et al. Aerosol composition and sources during the Chinese Spring Festival:fireworks, secondary aerosol, and holiday effects[J]. Atmospheric Chemistry and Physics Discussions,2014,14(14):20617-20646.
[27] Ramachandran S, Kedia S. Black carbon aerosols over an urban region:Radiative forcing and climate impact[J]. Journal of Geophysical Research, 2010,115(D10):1-11.
[28] Ran L, Deng Z Z, Wang P C, et al. Black carbon and wavelengthdependent aerosol absorption in the North China Plain based on two-year aethalometer measurements[J]. Atmospheric Environment, 2016,142:132-144.
[29]吴兑,毛节泰,邓雪娇,等.珠江三角洲黑碳气溶胶及其辐射特性的观测研究[J].中国科学(D辑:地球科学), 2009,39(11):1542-1553.Wu D, Mao J T, Deng X J, et al. Black carbon aerosols and their radiative properties in the Pearl River Delta region[J]. Sci China Ser D-Earth Sci, 2009,39(11):1542-1553.
[30] Drinovec L, Mo?nik G, Zotter P, et al. The"dual-spot"Aethalometer:an improved measurement of aerosol black carbon with real-time loading compensation[J]. Atmospheric Measurement Techniques Discussions, 2014,7(9):10179-10220.
[31] Aki V, Timo M K, Risto H, et al. A simple procedure for correcting loading effects of aethalometer data[J]. Journal of the Air and Waste Management Association(1995), 2007,57(10):1214-1222.
[32] Lin C Q, Liu G, Lau A K H, et al. High-resolution satellite remote sensing of provincial PM2.5 trends in China from 2001 to 2015[J].Atmospheric Environment, 2018,180:110-116.
[33] Kirchstetter T W, Novakov T, Hobbs P V. Evidence that the spectral dependence of light absorption by aerosols is affected by organic carbon[J]. Journal of Geophysical Research:Atmospheres, 2004,109(D21):1-12.
[34] Sandradewi J, Prév?t A S H, Szidat S, et al. Using Aerosol Light Absorption Measurements for the Quantitative Determination of Wood Burning and Traffic Emission Contributions to Particulate Matter[J].Environmental Science and Technology, 2008,42(9):3316-3323.
[35] Zotter P, Herich H, Gysel M, et al. Evaluation of the absorption?ngstr?m exponents for traffic and wood burning in the Aethalometer based source apportionment using radio carbon measurements of ambient aerosol[J]. Atmospheric Chemistry and Physics Discussions,2016,17(6):1-29.
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