太原市冬季PM_(2.5)化学组分特征与来源解析
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摘要
为研究太原市城区冬季PM_(2.5)污染特征及来源,于2017年1月对PM_(2.5)及其化学组分(水溶性离子、碳组分和微量元素)、气态污染物(SO_2、NO_2)进行在线观测,结合气象数据,分析了清洁天和污染天PM_(2.5)及其化学组分特征,并利用正定矩阵因子分析法(positive matrix factorization,PMF)对PM_(2.5)进行来源解析.结果表明,2017年1月太原市城区污染天PM_(2.5)质量浓度(239. 92μg·m~(-3))为清洁天的5. 70倍,污染天PM_(2.5)主要化学组分SO_4~(2-)、NO_3~-、NH_4~+、Cl~-、OC和EC分别为清洁天的7. 04、5. 76、6. 51、5. 62、4. 06和4. 70倍;污染天硫的氧化速率(SOR)和氮的氧化速率(NOR)分别为0. 12和0. 19,明显高于清洁天,说明污染天二次转化程度更高; PMF解析结果显示,污染天二次源(35. 06%)、燃煤源(30. 19%)和机动车源(24. 25%)较清洁天分别增长18. 03%、7. 39%和2. 10%,说明太原市城区污染天在管控机动车和燃煤等一次排放源的基础上,更应该注意对二次源前体物的控制.
To study the characteristics and sources of PM_(2.5) pollution in Taiyuan urban area in winter,PM_(2.5) and its chemical components( water-soluble ions,carbon components,and trace elements) and gaseous pollutants( SO_2,NO_2) were monitored by online instruments in January 2017. Combined with meteorological data,the characteristics of PM_(2.5) and its chemical components were analyzed. Also,source apportionment of PM_(2.5) was conducted by using positive matrix factorization( PMF). The results showed that the mean mass concentration of PM_(2.5) on polluted days( 239. 92 μg·m~(-3)) was 5. 70 times as much as that on clean days. The concentrations of the main chemical components of PM_(2.5) on polluted days,SO_4~(2-),NO_3~-,NH_4~+,Cl~-,OC,and EC,were 7. 04,5. 76,6. 51,5. 62,4. 06,and 4. 70 times their respective values on clean days. The sulfur oxidation ratios( SOR) and the nitrogen oxidation ratios( NOR) on polluted days were 0. 12 and 0. 19,respectively,which were higher than those in clean days,indicating that secondary transformation was more significant on polluted days. The results of the PMF source apportionment showed that the contributions of secondary sources( 35. 06%),coal combustion( 30. 19%),and vehicle emissions( 24. 25%) were higher on polluted days than on clean days,with increases of 18. 03%,7. 39% and 2. 10%,respectively. Thus,air pollution control strategies should pay more attention to controlling secondary source precursors on the basis of controlling the primary emission sources on polluted days.
To study the characteristics and sources of PM_(2.5) pollution in Taiyuan urban area in winter,PM_(2.5) and its chemical components( water-soluble ions,carbon components,and trace elements) and gaseous pollutants( SO_2,NO_2) were monitored by online instruments in January 2017. Combined with meteorological data,the characteristics of PM_(2.5) and its chemical components were analyzed. Also,source apportionment of PM_(2.5) was conducted by using positive matrix factorization( PMF). The results showed that the mean mass concentration of PM_(2.5) on polluted days( 239. 92 μg·m~(-3)) was 5. 70 times as much as that on clean days. The concentrations of the main chemical components of PM_(2.5) on polluted days,SO_4~(2-),NO_3~-,NH_4~+,Cl~-,OC,and EC,were 7. 04,5. 76,6. 51,5. 62,4. 06,and 4. 70 times their respective values on clean days. The sulfur oxidation ratios( SOR) and the nitrogen oxidation ratios( NOR) on polluted days were 0. 12 and 0. 19,respectively,which were higher than those in clean days,indicating that secondary transformation was more significant on polluted days. The results of the PMF source apportionment showed that the contributions of secondary sources( 35. 06%),coal combustion( 30. 19%),and vehicle emissions( 24. 25%) were higher on polluted days than on clean days,with increases of 18. 03%,7. 39% and 2. 10%,respectively. Thus,air pollution control strategies should pay more attention to controlling secondary source precursors on the basis of controlling the primary emission sources on polluted days.
引文
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[2]王跃思,姚利,王莉莉,等. 2013年元月我国中东部地区强霾污染成因分析[J].中国科学:地球科学,2014,44(1):15-26.Wang Y S, Yao L, Wang L L, et al. Mechanism for the formation of the January 2013 heavy haze pollution episode over central and eastern China[J]. Science China Earth Sciences,2014,57(1):14-25.
[3]白志鹏,蔡斌彬,董海燕,等.灰霾的健康效应[J].环境污染与防治,2006,28(3):198-201.
[4]贺克斌,杨复沫,段凤魁,等.大气颗粒物与区域复合污染[M].北京:科学出版社,2011.
[5]郑玫,张延君,闫才青,等.中国PM2. 5来源解析方法综述[J].北京大学学报(自然科学版),2014,50(6):1141-1154.Zheng M,Zhang Y J,Yan C Q,et al. Review of PM2. 5source apportionment methods in China[J]. Acta Scientiarum Naturalium Universitatis Pekinensis,2014,50(6):1141-1154.
[6] Zhang Y,Huang W, Cai T Q, et al. Concentrations and chemical compositions of fine particles(PM2. 5)during haze and non-haze days in Beijing[J]. Atmospheric Research,2016,174-175:62-69.
[7] Sun Z Q,Mu Y J,Liu Y J,et al. A comparison study on airborne particles during haze days and non-haze days in Beijing[J]. Science of the Total Environment,2013,456-457:1-8.
[8]张程,于兴娜,安俊琳,等.南京北郊不同大气污染程度下气溶胶化学组分特征[J].环境科学,2017,38(12):4932-4942.Zhang C, Yu X N, An J L, et al. Aerosol chemical characteristics for different air pollution levels in north suburban Nanjing[J]. Environmental Science,2017,38(12):4932-4942.
[9] Zhang Q,Shen Z X,Cao J J,et al. Variations in PM2. 5,TSP,BC,and trace gases(NO2,SO2,and O3)between haze and non-haze episodes in winter over Xi'an,China[J]. Atmospheric Environment,2015,112:64-71.
[10] Tian S L, Pan Y P, Wang Y S. Size-resolved source apportionment of particulate matter in urban Beijing during haze and non-haze episodes[J]. Atmospheric Chemistry and Physics Discussions,2015,15(6):9405-9443.
[11] Sulong N A,Latif M T,Khan M F,et al. Source apportionment and health risk assessment among specific age groups during haze and non-haze episodes in Kuala Lumpur,Malaysia[J]. Science of the Total Environment,2017,601-602:556-570.
[12]王念飞,陈阳,郝庆菊,等.苏州市PM2. 5中水溶性离子的季节变化及来源分析[J].环境科学,2016,37(12):4482-4489.Wang N F,Chen Y,Hao Q J,et al. Seasonal variation and source analysis of the water-soluble inorganic ions in fine particulate matter in Suzhou[J]. Environmental Science,2016,37(12):4482-4489.
[13]周瑶瑶,马嫣,郑军,等.南京北郊冬季霾天PM2. 5水溶性离子的污染特征与消光作用研究[J].环境科学,2015,36(6):1926-1934.Zhou Y Y,Ma Y,Zheng J,et al. Pollution characteristics and light extinction effects of water-soluble ions in PM2. 5during winter hazy days at north suburban Nanjing[J]. Environmental Science,2015,36(6):1926-1934.
[14]贾小花,解静芳,马翔,等.太原市冬季PM2. 5水溶性组分污染特征分析[J].中国环境科学,2013,33(4):599-604.Jia X H,Xie J F,Ma X,et al. Analysis of water-soluble constituents in winter of PM2. 5in Taiyuan City[J]. China Environmental Science,2013,33(4):599-604.
[15] He Q S,Guo W D,Zhang G X,et al. Characteristics and seasonal variations of carbonaceous species in PM2. 5in Taiyuan,China[J]. Atmosphere,2015,6(6):850-862.
[16]曹玲娴,耿红,姚晨婷,等.太原市冬季灰霾期间大气细颗粒物化学成分特征[J].中国环境科学,2014,34(4):837-843.Cao L X,Geng H,Yao C T,et al. Investigation of chemical compositions of atmospheric fine particles during a wintertime haze episode in Taiyuan City[J]. China Environmental Science,2014,34(4):837-843.
[17] He Q S,Yan Y L,Guo L L,et al. Characterization and source analysis of water-soluble inorganic ionic species in PM2. 5in Taiyuan city,China[J]. Atmospheric Research,2017,184:48-55.
[18] Gao J,Peng X,Chen G,et al. Insights into the chemical characterization and sources of PM2. 5in Beijing at a 1-h time resolution[J]. Science of the Total Environment,2016,542:162-171.
[19] Liu J,Wu D,Fan S J,et al. A one-year,on-line,multi-site observational study on water-soluble inorganic ions in PM2. 5over the Pearl River Delta region,China[J]. Science of the Total Environment,2017,601-602:1720-1732.
[20] Liu B S,Yang J M,Yuan J,et al. Source apportionment of atmospheric pollutants based on the online data by using PMF and ME2 models at a megacity,China[J]. Atmospheric Research,2017,185:22-31.
[21] Paatero P, Tapper U. Positive matrix factorization:A nonnegative factor model with optimal utilization of error estimates of data values[J]. Environmetrics,1994,5(2):111-126.
[22] Paatero P,Hopke P K. Rotational tools for factor analytic models[J]. Journal of Chemometrics,2009,23(2):91-100.
[23] Brown S G,Eberly S,Paatero P,et al. Methods for estimating uncertainty in PMF solutions:Examples with ambient air and water quality data and guidance on reporting PMF results[J].Science of the Total Environment,2015,518-519:626-635.
[24] Qiu X H,Duan L,Gao J,et al. Chemical composition and source apportionment of PM10and PM2. 5in different functional areas of Lanzhou,China[J]. Journal of Environmental Science,2016,40:75-83.
[25]李艳红,赵彩萍,荆肖军,等.太原地区灰霾天气特征及影响因子分析[J].气候与环境研究,2014,19(2):200-208.Li Y H,Zhao C P,Jing X J,et al. Characteristics of dust haze in Taiyuan and its causative factors[J]. Climatic and Environmental Research,2014,19(2):200-208.
[26] Han B,Zhang R,Yang W,et al. Heavy haze episodes in Beijing during January 2013:Inorganic ion chemistry and source analysis using highly time-resolved measurements from an urban site[J]. Science of the Total Environment,2016,544:319-329.
[27]元洁,刘保双,程渊,等. 2017年1月天津市区PM2. 5化学组分特征及高时间分辨率来源解析研究[J].环境科学学报,2018,38(3):1090-1101.Yuan J,Liu B S,Cheng Y,et al. Study on characteristics of PM2. 5and chemical components and source apportionment of high temporal resolution in January 2017 in Tianjin urban area[J].Acta Scientiae Circumstantiae,2018,38(3):1090-1101.
[28]汤莉莉,汤蕾,花艳,等.苏南三市秋冬季PM2. 5中水溶性离子和元素特征及源解析[J].大气科学学报,2015,38(5):686-693.Tang L L,Tang L,Hua Y,et al. Characteristics and source apportionment of water-soluble ions and elements in PM2. 5in three cities of South Jiangsu in autumn and winter[J].Transactions of Atmospheric Sciences,2015,38(5):686-693.
[29]沙丹丹,王红磊,朱彬,等.冬季PM2. 5中含碳气溶胶的污染特征——长江三角洲地区一次区域重污染过程分析[J].中国环境科学,2017,37(10):3611-3622.Sha D D,Wang H L,Z B,et al. Pollution characteristics of carbonaceous aerosols in PM2. 5during a regional heavy air pollution episode in winter in the Yangtze River Delta[J]. China Environmental Science,2017,37(10):3611-3622.
[30] Ohta S,Okita T. A chemical characterization of atmospheric aerosol in Sapporo[J]. Atmospheric Environment. Part A.General Topics,1990,24(4):815-822.
[31] Zhang R,Sun X S,Shi A J,et al. Secondary inorganic aerosols formation during haze episodes at an urban site in Beijing,China[J]. Atmospheric Environment,2018,177:275-282.
[32] Seinfeld J H,Pandis S N,Noone K. Atmospheric chemistry and physics:From air pollution to climate change[M]. New York:Wiley,1998.
[33] Tan T Y,Hu M,Li M R,et al. New insight into PM2. 5pollution patterns in Beijing based on one-year measurement of chemical compositions[J]. Science of the Total Environment,2018,621:734-743.
[34] Wang Y,Zhuang G S,Tang A H,et al. The ion chemistry and the source of PM2. 5aerosol in Beijing[J]. Atmospheric Environment,2005,39(21):3771-3784.
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