广州PM_(2.5)化学组分特征及其与气象因子的关系
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摘要
于2012年12月—2013年12月在广州城区(市站)和东部郊区(九龙)开展为期一年的PM2.5样品采集,并同步收集气象因子和气态污染物质量浓度等数据.结果表明,PM2.5中主要化学组分为有机质(OM)和硫酸盐(SO2-4),分别占市站和九龙PM2.5质量浓度的49.4%和15.2%及57.0%和17.3%.碳质气溶胶(OM和EC)贡献接近50%,二次无机气溶胶(SO2-4、NO-3和NH+4总和,SIA)贡献超过30%.由于以机动车尾气为代表的移动污染源在城市区域贡献较大,市站[NO-3]/[SO2-4]比值显著高于九龙.两个站点[NH+4]/[SO2-4]摩尔质量比均高于1.5,表明观测期间广州市干季大气处于富铵状态.市站和九龙站硫氧化率(SOR)和氮氧化率(NOR)的时空变化趋势与O3类似,表明大气光化学过程是影响广州市SOR和NOR的重要因素.相对湿度低于65%时,SOR和NOR均较高;温度对SOR和NOR的影响有显著的城郊差异.降雨对PM2.5及各化学组分浓度有显著去除作用.
In order to characterize major composition of PM2.5 and study its relations with meteorological factors in Guangzhou,we conducted one-year sampling from December 2012 to December 2013 at one urban site and one rural site,respectively. We analyzed water soluble ions,OC and EC in PM2.5.Gaseous pollutants( SO2, NO2, O3) and meteorological factors( temperature, relative humidity, rainfall precipitation) were also recorded simultaneously. Our results showed that organic matter( OM) and sulfate( SO2-4) were the major components in PM2.5 at the two sites. Carbonaceous aerosols( OM and EC) contributed about 50% of PM2.5 and secondary inorganic aerosols( SO2-4,NO-3 and NH+4) accounted for more than 30%. Higher[NO-3]/[SO2-4]ratios were observed at the urban site,probably due to more influence of vehicle exhausts in urban area. The ratios of[NH+4]to[SO2-4]were higher than 1.5 at the two sites,suggesting ammonium-rich atmosphere in Guangzhou during our dry-season campaign. The spatial and seasonal trends of sulfur oxidation ratio( SOR) and nitrogen oxidation ratio( NOR) were consistent with those of O3,which indicated that photochemistry could significantly affect sulfate and nitrate formation in the air of Guangzhou. We also found that SOR and NOR were both high under relative humidity below65%,while the impact of temperature on SOR and NOR was apparently different between urban and rural sites. Rainfall could efficiently remove PM2.5 and its major components.
In order to characterize major composition of PM2.5 and study its relations with meteorological factors in Guangzhou,we conducted one-year sampling from December 2012 to December 2013 at one urban site and one rural site,respectively. We analyzed water soluble ions,OC and EC in PM2.5.Gaseous pollutants( SO2, NO2, O3) and meteorological factors( temperature, relative humidity, rainfall precipitation) were also recorded simultaneously. Our results showed that organic matter( OM) and sulfate( SO2-4) were the major components in PM2.5 at the two sites. Carbonaceous aerosols( OM and EC) contributed about 50% of PM2.5 and secondary inorganic aerosols( SO2-4,NO-3 and NH+4) accounted for more than 30%. Higher[NO-3]/[SO2-4]ratios were observed at the urban site,probably due to more influence of vehicle exhausts in urban area. The ratios of[NH+4]to[SO2-4]were higher than 1.5 at the two sites,suggesting ammonium-rich atmosphere in Guangzhou during our dry-season campaign. The spatial and seasonal trends of sulfur oxidation ratio( SOR) and nitrogen oxidation ratio( NOR) were consistent with those of O3,which indicated that photochemistry could significantly affect sulfate and nitrate formation in the air of Guangzhou. We also found that SOR and NOR were both high under relative humidity below65%,while the impact of temperature on SOR and NOR was apparently different between urban and rural sites. Rainfall could efficiently remove PM2.5 and its major components.
引文
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孟晓艳. 2009. 北京及其周边地区冬季SO2的变化与输送特征[J]. 气候与环境研究,14(3):309-317
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Pathak R K, Yao X, Laura A K H, et al. 2003. Acidity and concentrations of ionic species of PM2.5 in Hong Kong [J].Atmospheric Environment, 37(8):1113-1124
Pathak R K, Wu W S, Wang T. 2009. Summertime PM2.5 ionic species in four major cities of China: nitrate formation in an ammonia-deficient atmosphere [J]. Atmospheric chemistry and Physics, 9(5): 1711-1722
施洋. 2014. 上海市亚微米级颗粒物(PM1)污染特征与霾污染机制[D]. 上海:复旦大学
Tao J, Zhang L M, Cao J J, et al. 2017. A review of current knowledge concerning PM2.5 chemical composition, aerosol optical properties and their relationships across China[J]. Atmospheric Chemistry & Physics, 17(15):9485-9518
Wang X, Ding X, Fu X, et al. 2012. Aerosol scattering coefficients and major chemical compositions of fine particles observed at a rural site hit the central Pearl River Delta, South China[J]. Journal of Environmental Science-china, 24(1):72-77
Wang H, An J, Cheng M, et al. 2016a. One year online measurements of water-soluble ions at the industrially polluted town of Nanjing, China: Sources seasonal and diurnal variations[J]. Chemosphere, 148:526-536
Wang T, Tham Y J, Xue L, et al. 2016b. Observations of nitryl chloride and modeling its source and effect on ozone in the planetary boundary layer of southern China[J]. Journal of Geophysical Research: Atmospheres, 121(5):2476-2489
王珉,胡敏. 2000. 青岛沿海大气气溶胶中海盐源的贡献[J]. 环境科学:21(5):83-85
Yu J Z, Huang X F, Xu J, et al. 2004. When aerosol sulfate goes up, so does oxalate: Implication for the formation mechanisms of oxalate. Environmental Science & Technology, 39(1):128-133
Wise E K,Comrie A C.2005. Meteorologically adjusted urban air quality trends in the Southwestern United States [J].Atmospheric Environment, 39:2969-2980
吴兑. 2012. 近十年中国灰霾天气研究综述[J]. 环境科学学报,32(2):257-269
郇宁,曾立民,邵敏. 2005. 气溶胶中有机碳及元素碳分析方法进展[J]. 北京大学学报(自然科学版),41(1):957-964
周一敏,赵昕奕. 2017. 北京地区 PM2.5浓度与气象要素的相关分析[J]. 北京大学学报(自然科学版),53(1):111-124
Zhang Y L, Cao F. 2015. Fine particulate matter (PM2.5) in China at a city level[J]. Aerosol & Air Quality Research, 17(3):730-740
Arthur T. DeGaetano, Owen M. Doherty. 2004. Temporal, spatial and meteorological variations in hourly PM2.5 concentration extremes in New York City [J]. Atmospheric Environment, 38:1547-1558
付晓辛. 2015. 珠江三角洲地区PM2.5浓度组成变化及其对粒子酸度和消光的影响[D].北京: 中国科学院广州地球化学研究所
高佳琦.2010. 深圳市大学城大气颗粒物(PM2.5)污染特征分析及源解析[D]. 哈尔滨:哈尔滨工业大学
He K, zhao Q, Ma Y, et al. 2012. Spatial and seasonal variability of PM2.5 acidity at two Chinese megacities: insights into the formation of secondary inorganic aerosol [J]. Atmospheric Chemistry and Physics, 12(3): 1377-1395
Huang X, Qiu R, Chak K, et al. 2011, Evidence of high PM2.5 strong acidity in ammonia-rich atmosphere of Guangzhou, China: Transition in pathways of ambient ammonia to form aerosol ammonium at [NH【math250z】]/[SO【math251z】]=1.5[J]. Atmospheric Research, 99 (3/4):488-495
廖碧婷,吴兑,常越,等. 2014. 广州地区SO【math252z】、NO【math253z】、NH【math254z】与相关气体污染特征研究[J]. 环境科学学报,34(6):1551-1559
刘寿东,张莉,张园园,等. 2018. 温湿度对南京北郊PM2.5中二次无机离子生成演化的影响[J]. 生态环境学报. 27(4):714-721
吕文英,徐海娟,王新明.2010.广州城区秋季大气PM2.5中主要水溶性无机离子分析[J].环境科学与技术,33(1):98-101
孟晓艳. 2009. 北京及其周边地区冬季SO2的变化与输送特征[J]. 气候与环境研究,14(3):309-317
马莹,吴兑,刘建,等.2017.广州干湿季典型灰霾过程水溶性离子成分对比分析[J].环境科学学报,37(1):73-81
潘洪密,吴兑,李菲,等.2015.广州地区大气能见度与颗粒物关系的初探[J].环境监控与预警,7(1):32-33
Pathak R K, Yao X, Laura A K H, et al. 2003. Acidity and concentrations of ionic species of PM2.5 in Hong Kong [J].Atmospheric Environment, 37(8):1113-1124
Pathak R K, Wu W S, Wang T. 2009. Summertime PM2.5 ionic species in four major cities of China: nitrate formation in an ammonia-deficient atmosphere [J]. Atmospheric chemistry and Physics, 9(5): 1711-1722
施洋. 2014. 上海市亚微米级颗粒物(PM1)污染特征与霾污染机制[D]. 上海:复旦大学
Tao J, Zhang L M, Cao J J, et al. 2017. A review of current knowledge concerning PM2.5 chemical composition, aerosol optical properties and their relationships across China[J]. Atmospheric Chemistry & Physics, 17(15):9485-9518
Wang X, Ding X, Fu X, et al. 2012. Aerosol scattering coefficients and major chemical compositions of fine particles observed at a rural site hit the central Pearl River Delta, South China[J]. Journal of Environmental Science-china, 24(1):72-77
Wang H, An J, Cheng M, et al. 2016a. One year online measurements of water-soluble ions at the industrially polluted town of Nanjing, China: Sources seasonal and diurnal variations[J]. Chemosphere, 148:526-536
Wang T, Tham Y J, Xue L, et al. 2016b. Observations of nitryl chloride and modeling its source and effect on ozone in the planetary boundary layer of southern China[J]. Journal of Geophysical Research: Atmospheres, 121(5):2476-2489
王珉,胡敏. 2000. 青岛沿海大气气溶胶中海盐源的贡献[J]. 环境科学:21(5):83-85
Yu J Z, Huang X F, Xu J, et al. 2004. When aerosol sulfate goes up, so does oxalate: Implication for the formation mechanisms of oxalate. Environmental Science & Technology, 39(1):128-133
Wise E K,Comrie A C.2005. Meteorologically adjusted urban air quality trends in the Southwestern United States [J].Atmospheric Environment, 39:2969-2980
吴兑. 2012. 近十年中国灰霾天气研究综述[J]. 环境科学学报,32(2):257-269
郇宁,曾立民,邵敏. 2005. 气溶胶中有机碳及元素碳分析方法进展[J]. 北京大学学报(自然科学版),41(1):957-964
周一敏,赵昕奕. 2017. 北京地区 PM2.5浓度与气象要素的相关分析[J]. 北京大学学报(自然科学版),53(1):111-124
Zhang Y L, Cao F. 2015. Fine particulate matter (PM2.5) in China at a city level[J]. Aerosol & Air Quality Research, 17(3):730-740