沈阳市采暖期与非采暖期空气PM_(2.5)污染特征及来源分析
|
摘要
为了研究沈阳市采暖期与非采暖期空气PM_(2.5)污染特征及来源,于2015年1月29日～2016年1月26日在沈阳市采集PM_(2.5)有效样品113组,并分析了其载带的水溶性离子、碳组分及元素组分.结果表明,采样期间沈阳市PM_(2.5)质量浓度均值为66μg·m~(-3),其中31. 0%的样品超过《环境空气质量标准》(GB 3095-2012)日均值二级标准(75μg·m~(-3)),采暖期PM_(2.5)的平均浓度和超标率(90μg·m~(-3)、68. 6%)明显高于非采暖期(51μg·m~(-3)、31. 4%).采样期间21种元素(除了Mg、Ti、Ca、Fe、Si)、水溶性离子(除Ca~(2+)以外)和OC、EC质量浓度均呈现出采暖期高于非采暖期的趋势;[NO_3~-]/[SO_4~(2-)]比值表明非采暖期受移动源影响明显增加,燃煤等固定源仍是采暖期PM_(2.5)的主要来源,PM_(2.5)中水溶性离子是固定源和移动源共同作用的结果;氮氧化率(NOR)和硫氧化率(SOR)分析得到NO_x二次转化程度较弱,SO_2二次转化程度较强,特别是在非采暖期;富集因子结果表明EF值较高的元素主要来自燃煤、交通污染和工业排放. PM_(2.5)组分重构质量与实测质量呈现较好的相关性,采暖期和非采暖期PM_(2.5)中主要组分均为有机物(OM 28. 0%、23. 1%)、矿物尘(MIN 14. 5%、26. 0%)和SO_4~(2-)(15. 1%、19. 9%),PM_(2.5)受二次粒子、燃烧源和扬尘源影响较大.
To study the atmospheric PM_(2.5) pollution characteristics and sources in heating and non-heating periods in Shenyang,113 groups of effective PM_(2.5) samples were collected from January 29,2015 to January 26,2016,and the water-soluble ions,carbon constituents and elements in PM_(2.5) were tested. The results indicated that the average PM_(2.5) mass concentration in Shenyang during the sampling period was 66 μg·m~(-3). Among the sampled PM_(2.5) concentrations,31. 0% exceeded the daily value of the secondary standard limit of the Chinese National Ambient Air Quality Standard( 75 μg·m~(-3)). The average concentration and over-standard rate of PM_(2.5) in the heating period( 90 μg·m~(-3),68. 6%) was higher than that of the non-heating period( 51 μg·m~(-3),31. 4%). The concentrations of the 21 elements( except Mg,Ti,Ca,Fe,and Si),water-soluble ions( except Ca~(2+)),OC,and EC were all higher in the heating period than in the non-heating period. The ratio of [NO_3~-]/[SO_4~(2-)]showed that the influence of moving source increased obviously in the non-heating period,and fixed source was still the main contributor in the heating period. The water-soluble ions were the result of the interaction of fixed source and moving source. The NOR and SOR analyses showed that the secondary conversion of NO_x was weak,and the secondary conversion of SO_2 was obvious,especially in the non-heating period. The enrichment factor showed that the elements with high EF value mainly came from coal burning,traffic pollution,and industrial emissions. The reconstructed PM_(2.5) masses were highly correlated with the measured ones. The main constituents of PM_(2.5) in both heating and non-heating seasons were organic matter( 28. 0%,23. 1%),mineral dust( 14. 5%,26. 0%),and sulfate( 15. 1%,19. 9%),and PM_(2.5) was mainly affected by the secondary particles,combustion sources and dust sources.
To study the atmospheric PM_(2.5) pollution characteristics and sources in heating and non-heating periods in Shenyang,113 groups of effective PM_(2.5) samples were collected from January 29,2015 to January 26,2016,and the water-soluble ions,carbon constituents and elements in PM_(2.5) were tested. The results indicated that the average PM_(2.5) mass concentration in Shenyang during the sampling period was 66 μg·m~(-3). Among the sampled PM_(2.5) concentrations,31. 0% exceeded the daily value of the secondary standard limit of the Chinese National Ambient Air Quality Standard( 75 μg·m~(-3)). The average concentration and over-standard rate of PM_(2.5) in the heating period( 90 μg·m~(-3),68. 6%) was higher than that of the non-heating period( 51 μg·m~(-3),31. 4%). The concentrations of the 21 elements( except Mg,Ti,Ca,Fe,and Si),water-soluble ions( except Ca~(2+)),OC,and EC were all higher in the heating period than in the non-heating period. The ratio of [NO_3~-]/[SO_4~(2-)]showed that the influence of moving source increased obviously in the non-heating period,and fixed source was still the main contributor in the heating period. The water-soluble ions were the result of the interaction of fixed source and moving source. The NOR and SOR analyses showed that the secondary conversion of NO_x was weak,and the secondary conversion of SO_2 was obvious,especially in the non-heating period. The enrichment factor showed that the elements with high EF value mainly came from coal burning,traffic pollution,and industrial emissions. The reconstructed PM_(2.5) masses were highly correlated with the measured ones. The main constituents of PM_(2.5) in both heating and non-heating seasons were organic matter( 28. 0%,23. 1%),mineral dust( 14. 5%,26. 0%),and sulfate( 15. 1%,19. 9%),and PM_(2.5) was mainly affected by the secondary particles,combustion sources and dust sources.
引文
[1]曹军骥.PM2.5与环境[M].北京:科学出版社,2014.5-8,193-197.
[2]Zhang X Y,Wang J Z,Wang Y Q,et al.Changes in chemical components of aerosol particles in different haze regions in China from 2006 to 2013 and contribution of meteorological factors[J].Atmospheric Chemistry and Physics,2015,15(22):12935-12952.
[3]陈瑞敏,吴雁,康文英,等.连续雾霾天气污染物浓度变化及天气形势特征分析[J].气候与环境研究,2014,19(2):209-218.Chen R M,Wu Y,Kang W Y,et al.Analysis of pollutant concentrations and characteristics of continuous smoggy weather[J].Climatic and Environmental Research,2014,19(2):209-218.
[4]刘庆阳,刘艳菊,杨峥,等.北京城郊冬季一次大气重污染过程颗粒物的污染特征[J].环境科学学报,2014,34(1):12-18.Liu Q Y,Liu Y J,Yang Z,et al.Daily variations of chemical properties in airborne particulate matter during a high pollution winter episode in Beijing[J].Acta Scientiae Circumstantiae,2014,34(1):12-18.
[5]张懿华,段玉森,高松,等.上海城区典型空气污染过程中细颗粒污染特征研究[J].中国环境科学,2011,31(7):1115-1121.Zhang Y H,Duan Y S,Gao S,et al.Characteristics of fine particulate matter during a typical air pollution episode in Shanghai urban area[J].China Environmental Science,2011,31(7):1115-1121.
[6]Lai S C,Zhao Y,Ding A J,et al.Characterization of PM2.5and the major chemical components during a 1-year campaign in rural Guangzhou,Southern China[J].Atmospheric Research,2016,167:208-215.
[7]Zhang J,Liu L,Wang Y Y,et al.Chemical composition,source,and process of urban aerosols during winter haze formation in Northeast China[J].Environmental Pollution,2017,231:357-366.
[8]马雁军,刘宁微,王扬锋,等.辽宁中部城市群大气环境研究进展[J].气象科技进展,2012,2(2):19-24.Ma Y J,Liu N W,Wang Y F,et al.Research advances on atmospheric environment research in multi-cities in the middle of Liaoning Province[J].Advances in Meteorological Science and Technology,2012,2(2):19-24.
[9]李晶,曲健,李哲,等.沈阳市环境空气PM2.5中有机碳、元素碳的污染特征研究[J].环境保护与循环经济,2018,38(1):50-54.
[10]Hong Y,Li C L,Li X L,et al.Analysis of compositional variation and source characteristics of water-soluble ions in PM2.5during several winter-haze pollution episodes in Shenyang,China[J].Atmosphere,2018,9(7):280.
[11]曲健,李晶,张晶,等.沈阳市城区采暖期PM2.5中水溶性离子的化学特征[J].中国环境监测,2015,31(5):57-60.Qu J,Li J,Zhang J,et al.Chemica character of water-soluble ions in PM2.5in Shenyang City during heating season[J].Environmental Monitoring in China,2015,31(5):57-60.
[12]杨复沫,段凤魁,贺克斌.PM2.5的化学物种采样与分析方法[J].中国环境监测,2004,20(5):14-20.Yang F M,Duan F K,He K B.PM2.5speciation sampling and analysis methods[J].Environmental Monitoring in China,2004,20(5):14-20.
[13]赵雪艳,谷超,杨焕明,等.新疆奎独乌区域冬季大气重污染过程PM2.5组成特征及来源解析[J].环境科学研究,2017,30(10):1515-1523.Zhao X Y,Gu C,Yang H M,et al.Chemical composition and source apportionment of PM2.5during a winter air pollution episode in the Kui-Du-Wu Area of Xinjiang Uygur Autonomous Region[J].Research of Environmental Sciences,2017,30(10):1515-1523.
[14]王新,聂燕,陈红,等.兰州城区大气PM2.5污染特征及来源解析[J].环境科学,2016,37(5):1619-1628.Wang X,Nie Y,Chen H,et al.Pollution characteristics and source apportionment of PM2.5in Lanzhou City[J].Environmental Science,2016,37(5):1619-1628.
[15]段云霞,李得勤,田莉,等.沈阳市一次持续性重污染天气过程特征分析[J].干旱气象,2016,34(5):803-810.Duan Y X,Li D Q,Tian L,et al.Characteristic analysis of a continuous and serious pollution weather process in Shenyang[J].Journal of Arid Meteorology,2016,34(5):803-810.
[16]李崇,袁子鹏,吴宇童,等.沈阳一次严重污染天气过程持续和增强气象条件分析[J].环境科学研究,2017,30(3):349-358.Li C,Yuan Z P,Wu Y T,et al.Analysis of persistence and intensification mechanism of a heavy haze event in Shenyang[J].Research of Environmental Sciences,2017,30(3):349-358.
[17]唐孝炎,张远航,邵敏.大气环境化学[M].(第二版).北京:高等教育出版社,2006.500-503.
[18]张云峰,于瑞莲,胡恭任,等.泉州市大气PM2.5中水溶性离子季节变化特征及来源解析[J].环境科学,2017,38(10):4044-4053.Zhang Y F,Yu R L,Hu G R,et al.Seasonal variation and source apportionment of water-soluble ions in PM2.5in Quanzhou City[J].Environmental Science,2017,38(10):4044-4053.
[19]Yao X H,Chan C K,Fang M,et al.The water-soluble ionic composition of PM2.5in Shanghai and Beijing,China[J].Atmospheric Environment,2002,36(26):4223-4234.
[20]刘保献,张大伟,陈添,等.北京市PM2.5主要化学组分浓度水平研究与特征分析[J].环境科学学报,2015,35(12):4053-4060.Liu B X,Zhang D W,Chen T,et al.Characteristics and major chemical compositions of PM2.5in Beijing[J].Acta Scientiae Circumstantiae,2015,35(12):4053-4060.
[21]Kim B M,Teffera S,Zeldin M D.Characterization of PM2.5and PM10in the south coast air basin of southern California:Part 1-spatial variations[J].Journal of the Air&Waste Management Association,2000,50(12):2034-2044.
[22]吴丹,蔺少龙,杨焕强,等.杭州市PM2.5中水溶性离子的污染特征及其消光贡献[J].环境科学,2017,38(7):2656-2666.Wu D,Lin S L,Yang H Q,et al.Pollution characteristics and light extinction contribution of water-soluble ions of PM2.5in Hangzhou[J].Environmental Science,2017,38(7):2656-2666.
[23]Wang P,Cao J J,Shen Z X,et al.Spatial and seasonal variations of PM2.5mass and species during 2010 in Xi'an,China[J].Science of the Total Environment,2015,508:477-487.
[24]申进朝,陈纯,多克辛.部分中原城市PM2.5中水溶性离子污染特征[J].环境科学与技术,2014,37(7):153-156.Shen J C,Chen C,Duo K X.Pollution characteristics of water soluble ions in PM2.5in some cities of central China[J].Environmental Science&Technology,2014,37(7):153-156.
[25]魏明娜,谢海燕,邓文叶,等.乌鲁木齐市采暖期与非采暖期大气PM2.5和PM10中水溶性离子特征分析[J].安全与环境学报,2017,17(5):1986-1991.Wei M N,Xie H Y,Deng W Y,et al.Water-soluble ions pollution characteristics of the atmospheric particles(PM2.5and PM10)in Urumqi during the heating and non-heating periods[J].Journal of Safety and Environment,2017,17(5):1986-1991.
[26]Ohta S,Okita T.A chemical characterization of atmospheric aerosol in Sapporo[J].Atmospheric Environment.Part A.General Topics,1990,24(4):815-822.
[27]Quan J N,Zhang X S,Zhang Q,et al.Importance of sulfate emission to sulfur deposition at urban and rural sites in China[J].Atmospheric Research,2008,89(3):283-288.
[28]Chow J C,Watson J G,Lu Z Q,et al.Descriptive analysis of PM2.5and PM10at regionally representative locations during SJVAQS/AUSPEX[J].Atmospheric Environment,1996,30(12):2079-2112.
[29]杨勇杰,王跃思,温天雪,等.采暖期开始前后北京大气颗粒物中化学元素特征及来源[J].环境科学,2008,29(11):3275-3279.Yang Y J,Wang Y S,Wen T X,et al.Characteristics and sources of elements of atmospheric particles before and in heating period in Beijing[J].Environmental Science,2008,29(11):3275-3279.
[30]白志鹏.空气颗粒物测量技术[M].北京:化学工业出版社,2014.149-150.
[31]国家环境保护局,中国环境监测总站.中国土壤元素背景值[J].北京:中国环境科学出版社,1990.
[32]Huang X D,Olmez I,Aras N K,et al.Emissions of trace elements from motor vehicles:potential marker elements and source composition profile[J].Atmospheric Environment,1994,28(8):1385-1391.
[33]王伟,孔少飞,刘海彪,等.南京市春节前后大气PM2.5中重金属来源及健康风险评价[J].中国环境科学,2016,36(7):2186-2195.Wang W,Kong S F,Liu H B,et al.Sources and risk assessment of heavy metals in PM2.5around 2014 Spring Festival in Nanjing[J].China Environmental Science,2016,36(7):2186-2195.
[34]Zhao M J,Zhang Y,Ma W C,et al.Characteristics and ship traffic source identification of air pollutants in China's largest port[J].Atmospheric Environment,2013,64:277-286.
[35]Tian S L,Pan Y P,Liu Z R,et al.Size-resolved aerosol chemical analysis of extreme haze pollution events during early2013 in urban Beijing,China[J].Journal of Hazardous Materials,2014,279:452-460.
[36]Frank N H.Retained nitrate,hydrated sulfates,and carbonaceous mass in federal reference method fine particulate matter for six eastern U.S.Cities[J].Air Repair,2006,56(4):500-511.
[2]Zhang X Y,Wang J Z,Wang Y Q,et al.Changes in chemical components of aerosol particles in different haze regions in China from 2006 to 2013 and contribution of meteorological factors[J].Atmospheric Chemistry and Physics,2015,15(22):12935-12952.
[3]陈瑞敏,吴雁,康文英,等.连续雾霾天气污染物浓度变化及天气形势特征分析[J].气候与环境研究,2014,19(2):209-218.Chen R M,Wu Y,Kang W Y,et al.Analysis of pollutant concentrations and characteristics of continuous smoggy weather[J].Climatic and Environmental Research,2014,19(2):209-218.
[4]刘庆阳,刘艳菊,杨峥,等.北京城郊冬季一次大气重污染过程颗粒物的污染特征[J].环境科学学报,2014,34(1):12-18.Liu Q Y,Liu Y J,Yang Z,et al.Daily variations of chemical properties in airborne particulate matter during a high pollution winter episode in Beijing[J].Acta Scientiae Circumstantiae,2014,34(1):12-18.
[5]张懿华,段玉森,高松,等.上海城区典型空气污染过程中细颗粒污染特征研究[J].中国环境科学,2011,31(7):1115-1121.Zhang Y H,Duan Y S,Gao S,et al.Characteristics of fine particulate matter during a typical air pollution episode in Shanghai urban area[J].China Environmental Science,2011,31(7):1115-1121.
[6]Lai S C,Zhao Y,Ding A J,et al.Characterization of PM2.5and the major chemical components during a 1-year campaign in rural Guangzhou,Southern China[J].Atmospheric Research,2016,167:208-215.
[7]Zhang J,Liu L,Wang Y Y,et al.Chemical composition,source,and process of urban aerosols during winter haze formation in Northeast China[J].Environmental Pollution,2017,231:357-366.
[8]马雁军,刘宁微,王扬锋,等.辽宁中部城市群大气环境研究进展[J].气象科技进展,2012,2(2):19-24.Ma Y J,Liu N W,Wang Y F,et al.Research advances on atmospheric environment research in multi-cities in the middle of Liaoning Province[J].Advances in Meteorological Science and Technology,2012,2(2):19-24.
[9]李晶,曲健,李哲,等.沈阳市环境空气PM2.5中有机碳、元素碳的污染特征研究[J].环境保护与循环经济,2018,38(1):50-54.
[10]Hong Y,Li C L,Li X L,et al.Analysis of compositional variation and source characteristics of water-soluble ions in PM2.5during several winter-haze pollution episodes in Shenyang,China[J].Atmosphere,2018,9(7):280.
[11]曲健,李晶,张晶,等.沈阳市城区采暖期PM2.5中水溶性离子的化学特征[J].中国环境监测,2015,31(5):57-60.Qu J,Li J,Zhang J,et al.Chemica character of water-soluble ions in PM2.5in Shenyang City during heating season[J].Environmental Monitoring in China,2015,31(5):57-60.
[12]杨复沫,段凤魁,贺克斌.PM2.5的化学物种采样与分析方法[J].中国环境监测,2004,20(5):14-20.Yang F M,Duan F K,He K B.PM2.5speciation sampling and analysis methods[J].Environmental Monitoring in China,2004,20(5):14-20.
[13]赵雪艳,谷超,杨焕明,等.新疆奎独乌区域冬季大气重污染过程PM2.5组成特征及来源解析[J].环境科学研究,2017,30(10):1515-1523.Zhao X Y,Gu C,Yang H M,et al.Chemical composition and source apportionment of PM2.5during a winter air pollution episode in the Kui-Du-Wu Area of Xinjiang Uygur Autonomous Region[J].Research of Environmental Sciences,2017,30(10):1515-1523.
[14]王新,聂燕,陈红,等.兰州城区大气PM2.5污染特征及来源解析[J].环境科学,2016,37(5):1619-1628.Wang X,Nie Y,Chen H,et al.Pollution characteristics and source apportionment of PM2.5in Lanzhou City[J].Environmental Science,2016,37(5):1619-1628.
[15]段云霞,李得勤,田莉,等.沈阳市一次持续性重污染天气过程特征分析[J].干旱气象,2016,34(5):803-810.Duan Y X,Li D Q,Tian L,et al.Characteristic analysis of a continuous and serious pollution weather process in Shenyang[J].Journal of Arid Meteorology,2016,34(5):803-810.
[16]李崇,袁子鹏,吴宇童,等.沈阳一次严重污染天气过程持续和增强气象条件分析[J].环境科学研究,2017,30(3):349-358.Li C,Yuan Z P,Wu Y T,et al.Analysis of persistence and intensification mechanism of a heavy haze event in Shenyang[J].Research of Environmental Sciences,2017,30(3):349-358.
[17]唐孝炎,张远航,邵敏.大气环境化学[M].(第二版).北京:高等教育出版社,2006.500-503.
[18]张云峰,于瑞莲,胡恭任,等.泉州市大气PM2.5中水溶性离子季节变化特征及来源解析[J].环境科学,2017,38(10):4044-4053.Zhang Y F,Yu R L,Hu G R,et al.Seasonal variation and source apportionment of water-soluble ions in PM2.5in Quanzhou City[J].Environmental Science,2017,38(10):4044-4053.
[19]Yao X H,Chan C K,Fang M,et al.The water-soluble ionic composition of PM2.5in Shanghai and Beijing,China[J].Atmospheric Environment,2002,36(26):4223-4234.
[20]刘保献,张大伟,陈添,等.北京市PM2.5主要化学组分浓度水平研究与特征分析[J].环境科学学报,2015,35(12):4053-4060.Liu B X,Zhang D W,Chen T,et al.Characteristics and major chemical compositions of PM2.5in Beijing[J].Acta Scientiae Circumstantiae,2015,35(12):4053-4060.
[21]Kim B M,Teffera S,Zeldin M D.Characterization of PM2.5and PM10in the south coast air basin of southern California:Part 1-spatial variations[J].Journal of the Air&Waste Management Association,2000,50(12):2034-2044.
[22]吴丹,蔺少龙,杨焕强,等.杭州市PM2.5中水溶性离子的污染特征及其消光贡献[J].环境科学,2017,38(7):2656-2666.Wu D,Lin S L,Yang H Q,et al.Pollution characteristics and light extinction contribution of water-soluble ions of PM2.5in Hangzhou[J].Environmental Science,2017,38(7):2656-2666.
[23]Wang P,Cao J J,Shen Z X,et al.Spatial and seasonal variations of PM2.5mass and species during 2010 in Xi'an,China[J].Science of the Total Environment,2015,508:477-487.
[24]申进朝,陈纯,多克辛.部分中原城市PM2.5中水溶性离子污染特征[J].环境科学与技术,2014,37(7):153-156.Shen J C,Chen C,Duo K X.Pollution characteristics of water soluble ions in PM2.5in some cities of central China[J].Environmental Science&Technology,2014,37(7):153-156.
[25]魏明娜,谢海燕,邓文叶,等.乌鲁木齐市采暖期与非采暖期大气PM2.5和PM10中水溶性离子特征分析[J].安全与环境学报,2017,17(5):1986-1991.Wei M N,Xie H Y,Deng W Y,et al.Water-soluble ions pollution characteristics of the atmospheric particles(PM2.5and PM10)in Urumqi during the heating and non-heating periods[J].Journal of Safety and Environment,2017,17(5):1986-1991.
[26]Ohta S,Okita T.A chemical characterization of atmospheric aerosol in Sapporo[J].Atmospheric Environment.Part A.General Topics,1990,24(4):815-822.
[27]Quan J N,Zhang X S,Zhang Q,et al.Importance of sulfate emission to sulfur deposition at urban and rural sites in China[J].Atmospheric Research,2008,89(3):283-288.
[28]Chow J C,Watson J G,Lu Z Q,et al.Descriptive analysis of PM2.5and PM10at regionally representative locations during SJVAQS/AUSPEX[J].Atmospheric Environment,1996,30(12):2079-2112.
[29]杨勇杰,王跃思,温天雪,等.采暖期开始前后北京大气颗粒物中化学元素特征及来源[J].环境科学,2008,29(11):3275-3279.Yang Y J,Wang Y S,Wen T X,et al.Characteristics and sources of elements of atmospheric particles before and in heating period in Beijing[J].Environmental Science,2008,29(11):3275-3279.
[30]白志鹏.空气颗粒物测量技术[M].北京:化学工业出版社,2014.149-150.
[31]国家环境保护局,中国环境监测总站.中国土壤元素背景值[J].北京:中国环境科学出版社,1990.
[32]Huang X D,Olmez I,Aras N K,et al.Emissions of trace elements from motor vehicles:potential marker elements and source composition profile[J].Atmospheric Environment,1994,28(8):1385-1391.
[33]王伟,孔少飞,刘海彪,等.南京市春节前后大气PM2.5中重金属来源及健康风险评价[J].中国环境科学,2016,36(7):2186-2195.Wang W,Kong S F,Liu H B,et al.Sources and risk assessment of heavy metals in PM2.5around 2014 Spring Festival in Nanjing[J].China Environmental Science,2016,36(7):2186-2195.
[34]Zhao M J,Zhang Y,Ma W C,et al.Characteristics and ship traffic source identification of air pollutants in China's largest port[J].Atmospheric Environment,2013,64:277-286.
[35]Tian S L,Pan Y P,Liu Z R,et al.Size-resolved aerosol chemical analysis of extreme haze pollution events during early2013 in urban Beijing,China[J].Journal of Hazardous Materials,2014,279:452-460.
[36]Frank N H.Retained nitrate,hydrated sulfates,and carbonaceous mass in federal reference method fine particulate matter for six eastern U.S.Cities[J].Air Repair,2006,56(4):500-511.
© 2004-2018 中国地质图书馆版权所有 京ICP备05064691号 京公网安备11010802017129号 地址：北京市海淀区学院路29号 邮编：100083 电话：办公室：(+86 10)66554848；文献借阅、咨询服务、科技查新：66554700 |