郑州市大气细颗粒物中水溶性离子季节性变化特征及其源解析
|
摘要
为探究郑州市PM_(2.5)的污染水平,水溶性离子组成特征并进行来源分析,于2016年四季进行PM_(2.5)周年膜采样,每个季节连续采集30 d共采集有效样品170个.分别采用重量法测定PM_(2.5)的质量浓度,离子色谱法测定水溶性离子浓度,并使用主成分分析法对其进行来源解析.结果表明,在采样期间郑州市PM_(2.5)年均质量浓度为150. 72μg·m~(-3),季节性特征明显,冬季最高,夏季最低,秋季略高于春季. NH_4~+、NO_3~-、SO_4~(2-)是郑州PM_(2.5)中最主要的无机水溶性离子,三离子之和占所测7种水溶性离子总含量的比例分别为92. 55%(春)、92. 94%(夏)、93. 06%(秋)和93. 15%(冬).阴阳离子电荷当量年均值为0. 886,PM_(2.5)呈弱碱性.春、夏季节铵盐的存在形态为NH_4NO_3和(NH_4)_2SO_4,秋季铵盐的存在形式可能为NH_4NO_3、(NH_4)_2SO_4和NH_4HSO_4,冬季NH_4~+除上述3种存在形式外,可能还以NH_4Cl或其他形式存在.郑州市大气中存在较强的SO_2、NO_2二次转化过程,水溶性离子的主要来源是二次转化过程,化石燃料和生物质燃烧、矿尘、农业活动以及土壤和建筑尘等.
In order to explore the characteristics of PM_(2.5) concentration and water-soluble inorganic ions in Zhengzhou City,a total of170 PM_(2.5) samples were collected in the spring,summer,autumn,and winter seasons of 2016,with 30 days continuous sampling during each season. The mass concentration of PM_(2.5) was analyzed gravimetrically,water-soluble inorganic ions were determined by ion chromatography,and principle component analysis was employed for source apportionment. The results showed that the mass concentration of PM_(2.5) was 150. 72 μg·m~(-3) during the sampling period. The mass concentration was highest in winter and lowest in summer,and that of autumn is higher was higher than that of spring. The ions SO_4~(2-),NO_3~-,and NH_4~+were the major WSIs found in PM_(2.5),accounting for 92. 55%,92. 94%,93. 06%,and 93. 15% of the total amount of the seven ions found in spring,summer,autumn,and winter,respectively. The anion-to-cation ratio was 0. 886,which indicated that PM_(2.5) was slightly alkaline in Zhengzhou.Secondary inorganic species,including NH_4~+,NO_3~-,and SO_4~(2-)were the major components of the water-soluble ions. These ions most likely existed in the form of NH_4 NO_3 and( NH_4)_2 SO_4 during spring and summer,while they were present as NH_4 NO_3,( NH_4)_2 SO_4 and NH_4 HSO_4 in autumn. In addition to these three forms,NH_4 Cl or other forms may exist in winter. Industrial emissions,combustion,secondary transformation,soil,and construction dust were the major sources of the water-soluble ions in PM_(2.5).
In order to explore the characteristics of PM_(2.5) concentration and water-soluble inorganic ions in Zhengzhou City,a total of170 PM_(2.5) samples were collected in the spring,summer,autumn,and winter seasons of 2016,with 30 days continuous sampling during each season. The mass concentration of PM_(2.5) was analyzed gravimetrically,water-soluble inorganic ions were determined by ion chromatography,and principle component analysis was employed for source apportionment. The results showed that the mass concentration of PM_(2.5) was 150. 72 μg·m~(-3) during the sampling period. The mass concentration was highest in winter and lowest in summer,and that of autumn is higher was higher than that of spring. The ions SO_4~(2-),NO_3~-,and NH_4~+were the major WSIs found in PM_(2.5),accounting for 92. 55%,92. 94%,93. 06%,and 93. 15% of the total amount of the seven ions found in spring,summer,autumn,and winter,respectively. The anion-to-cation ratio was 0. 886,which indicated that PM_(2.5) was slightly alkaline in Zhengzhou.Secondary inorganic species,including NH_4~+,NO_3~-,and SO_4~(2-)were the major components of the water-soluble ions. These ions most likely existed in the form of NH_4 NO_3 and( NH_4)_2 SO_4 during spring and summer,while they were present as NH_4 NO_3,( NH_4)_2 SO_4 and NH_4 HSO_4 in autumn. In addition to these three forms,NH_4 Cl or other forms may exist in winter. Industrial emissions,combustion,secondary transformation,soil,and construction dust were the major sources of the water-soluble ions in PM_(2.5).
引文
[1] Ho K F,Lee S C,Chan C K,et al. Characterization of chemical species in PM2. 5and PM10aerosols in Hong Kong[J].Atmospheric Environment,2003,37(1):31-39.
[2] Calvo A I,Alves C,Castro A,et al. Research on aerosol sources and chemical composition:Past,current and emerging issues[J]. Atmospheric Research,2013,120-121:1-28.
[3] Li T C,Yuan C S,Huang H C,et al. Clustered long-range transport routes and potential sources of PM2. 5and their chemical characteristics around the Taiwan Strait[J]. Atmospheric Environment,2017,148:152-166.
[4] Huang T,Chen J,Zhao W T,et al. Seasonal variations and correlation analysis of water-soluble inorganic ions in PM2. 5in Wuhan,2013[J]. Atmosphere,2016,7(4):49.
[5]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.
[6]张棕巍,胡恭任,于瑞莲,等.厦门市大气PM2. 5中水溶性离子污染特征及来源解析[J].中国环境科学,2016,36(7):1947-1954.Zhang Z W,Hu G R,Yu R L,et al. Characteristics and sources apportionment of water-soluble ions in PM2. 5of Xiamen City,China[J]. China Environmental Science,2016,36(7):1947-1954.
[7] Liu P F,Zhang C L,Mu Y J,et al. The possible contribution of the periodic emissions from farmers'activities in the North China Plain to atmospheric water-soluble ions in Beijing[J].Atmospheric Chemistry and Physics,2016,16(15):10097-10109.
[8]郭送军,谭吉华,段菁春,等.广州市灰霾期大气PM10中水溶性离子特征[J].环境科学与技术,2012,35(11):83-86.Guo S J,Tan J H,Duan J C,et al. Characteristics of water soluble ions in atmospheric PM10during haze periods in Guangzhou[J]. Environmental Science&Technology,2012,35(11):83-86.
[9]郭新彪,魏红英.大气PM2. 5对健康影响的研究进展[J].科学通报,2013,58(13):1171-1177.Guo X B,Wei H Y. Progress on the health effects of ambient PM2. 5pollution[J]. Chinese Science Bulletin,2013,58(13):1171-1177.
[10]殷永文,程金平,段玉森,等.上海市霾期间PM2. 5、PM10污染与呼吸科、儿呼吸科门诊人数的相关分析[J].环境科学,2011,32(7):1894-1898.Yin Y W,Cheng J P,Duan Y S,et al. Correlation analysis between the PM2. 5,PM10which were taken in the hazy day and the number of outpatient about breathing sections, breathing sections of pediatrics in Shanghai[J]. Environmental Science,2011,32(7):1894-1898.
[11] 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.
[12] Zhang T,Cao J J,Tie X X,et al. Water-soluble ions in atmospheric aerosols measured in Xi'an, China:Seasonal variations and sources[J]. Atmospheric Research,2011,102(1-2):110-119.
[13]杨懂艳,刘保献,张大伟,等. 2012~2013年间北京市PM2. 5中水溶性离子时空分布规律及相关性分析[J].环境科学,2015,36(3):768-773.Yang D Y,Liu B X,Zhang D W,et al. Correlation,seasonal and temporal variation of water-soluble ions of PM2. 5in Beijing during 2012-2013[J]. Environmental Science,2015,36(3):768-773.
[14]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.
[15] Geng N B,Wang J,Xu Y F,et al. PM2. 5in an industrial district of Zhengzhou,China:chemical composition and source apportionment[J]. Particuology,2013,11(1):99-109.
[16]杨书申,宋晓焱,郑明凯,等.郑州市灰霾天气过程PM2. 5水溶性无机离子污染分析[J].安全与环境学报,2016,16(6):348-353.Yang S S,Song X Y,Zheng M K,et al. Characteristic features of the water-soluble inorganic ions in PM2. 5in the process of a severe haze episode in Zhengzhou[J]. Journal of Safety and Environment,2016,16(6):348-353.
[17] HJ 656-2013,环境空气颗粒物(PM2. 5)手工监测方法(重量法)技术规范[S].
[18]贾佳,韩力慧,程水源,等.京津冀区域PM2. 5及二次无机组分污染特征研究[J].中国环境科学,2018,38(3):801-811.Jia J,Han L H,Cheng S Y,et al. Pollution characteristic of PM2. 5and secondary inorganic ions in Beijing-Tianjin-Hebei region[J]. China Environmental Science,2018,38(3):801-811.
[19]李凤菊,邵龙义,杨书申,等.郑州大气PM10的形貌特征及生物活性研究[J].环境科学,2008,29(9):2654-2658.Li F J,Shao L Y,Yang S S,et al. Morphology and bioreactivity of PM10in air of Zhengzhou[J]. Environmental Science,2008,29(9):2654-2658.
[20]郭家瑜,张英杰,郑海涛,等.北京2015年大气细颗粒物的空间分布特征及变化规律[J].环境科学学报,2017,37(7):2409-2419.Guo J Y,Zhang Y J,Zheng H T,et al. Characteristics of spatial distribution and variations of atmospheric fine particles in Beijing in 2015[J]. Acta Scientiae Circumstantiae,2017,37(7):2409-2419.
[21]吕佳莉,李萌,解静芳,等.太原城区PM2. 5重金属元素季节变化及形态分析[J].环境科学与技术,2016,39(4):126-131.Lyu J L,Li M,Xie J F,et al. Seasonal variation and chemical speciation analysis of heavy metal pollution in PM2. 5from urban area of Taiyuan[J]. Environmental Science&Technology,2016,39(4):126-131.
[22]王佳,李晓,吴瑞杰,等.郑州市PM2. 5和PM10中水溶性无机离子的污染特征[J].郑州大学学报(理学版),2014,46(4):81-87.Wang J,Li X,Wu R J,et al. Pollution characteristics of watersoluble ions in PM2. 5and PM10in Zhengzhou[J]. Journal of Zhengzhou University(Natural Science Edition),2014,46(4):81-87.
[23] Wang H L,Qiao L P,Lou S R,et al. Chemical composition of PM2. 5and meteorological impact among three years in urban Shanghai,China[J]. Journal of Cleaner Production,2016,112:1302-1311.
[24]吴耕晨.广州大气气溶胶水溶性组分分布特征的研究[D].广州:暨南大学,2015.Wu G C. Analysis of distribution characteristics for water soluble content in aerosol in Guangzhou[D]. Guangzhou:Jinan University,2015.
[25] Xu L L,Chen X Q,Chen J S,et al. Seasonal variations and chemical compositions of PM2. 5aerosol in the urban area of Fuzhou,China[J]. Atmospheric Research,2012,104-105:264-272.
[26]冯加良,胡小玲,管晶晶,等.上海市大气细颗粒物的酸度及其与组成的关系[J].上海大学学报(自然科学版),2010,16(5):431-436.Feng J L,Hu X L,Guan J J,et al. Acidity of PM2. 5in Shanghai and its correlation with chemical composition of the particles[J].Journal of Shanghai University(Natural Science),2010,16(5):431-436.
[27] Shon Z H,Ghosh S,Kim K H,et al. Analysis of water-soluble ions and their precursor gases over diurnal cycle[J].Atmospheric Research,2013,132-133:309-321.
[28] Han Y M,Du P X,Cao J J,et al. Multivariate analysis of heavy metal contamination in urban dusts of Xi'an,Central China[J].Science of the Total Environment,2006,355(1-3):176-186.
[2] Calvo A I,Alves C,Castro A,et al. Research on aerosol sources and chemical composition:Past,current and emerging issues[J]. Atmospheric Research,2013,120-121:1-28.
[3] Li T C,Yuan C S,Huang H C,et al. Clustered long-range transport routes and potential sources of PM2. 5and their chemical characteristics around the Taiwan Strait[J]. Atmospheric Environment,2017,148:152-166.
[4] Huang T,Chen J,Zhao W T,et al. Seasonal variations and correlation analysis of water-soluble inorganic ions in PM2. 5in Wuhan,2013[J]. Atmosphere,2016,7(4):49.
[5]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.
[6]张棕巍,胡恭任,于瑞莲,等.厦门市大气PM2. 5中水溶性离子污染特征及来源解析[J].中国环境科学,2016,36(7):1947-1954.Zhang Z W,Hu G R,Yu R L,et al. Characteristics and sources apportionment of water-soluble ions in PM2. 5of Xiamen City,China[J]. China Environmental Science,2016,36(7):1947-1954.
[7] Liu P F,Zhang C L,Mu Y J,et al. The possible contribution of the periodic emissions from farmers'activities in the North China Plain to atmospheric water-soluble ions in Beijing[J].Atmospheric Chemistry and Physics,2016,16(15):10097-10109.
[8]郭送军,谭吉华,段菁春,等.广州市灰霾期大气PM10中水溶性离子特征[J].环境科学与技术,2012,35(11):83-86.Guo S J,Tan J H,Duan J C,et al. Characteristics of water soluble ions in atmospheric PM10during haze periods in Guangzhou[J]. Environmental Science&Technology,2012,35(11):83-86.
[9]郭新彪,魏红英.大气PM2. 5对健康影响的研究进展[J].科学通报,2013,58(13):1171-1177.Guo X B,Wei H Y. Progress on the health effects of ambient PM2. 5pollution[J]. Chinese Science Bulletin,2013,58(13):1171-1177.
[10]殷永文,程金平,段玉森,等.上海市霾期间PM2. 5、PM10污染与呼吸科、儿呼吸科门诊人数的相关分析[J].环境科学,2011,32(7):1894-1898.Yin Y W,Cheng J P,Duan Y S,et al. Correlation analysis between the PM2. 5,PM10which were taken in the hazy day and the number of outpatient about breathing sections, breathing sections of pediatrics in Shanghai[J]. Environmental Science,2011,32(7):1894-1898.
[11] 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.
[12] Zhang T,Cao J J,Tie X X,et al. Water-soluble ions in atmospheric aerosols measured in Xi'an, China:Seasonal variations and sources[J]. Atmospheric Research,2011,102(1-2):110-119.
[13]杨懂艳,刘保献,张大伟,等. 2012~2013年间北京市PM2. 5中水溶性离子时空分布规律及相关性分析[J].环境科学,2015,36(3):768-773.Yang D Y,Liu B X,Zhang D W,et al. Correlation,seasonal and temporal variation of water-soluble ions of PM2. 5in Beijing during 2012-2013[J]. Environmental Science,2015,36(3):768-773.
[14]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.
[15] Geng N B,Wang J,Xu Y F,et al. PM2. 5in an industrial district of Zhengzhou,China:chemical composition and source apportionment[J]. Particuology,2013,11(1):99-109.
[16]杨书申,宋晓焱,郑明凯,等.郑州市灰霾天气过程PM2. 5水溶性无机离子污染分析[J].安全与环境学报,2016,16(6):348-353.Yang S S,Song X Y,Zheng M K,et al. Characteristic features of the water-soluble inorganic ions in PM2. 5in the process of a severe haze episode in Zhengzhou[J]. Journal of Safety and Environment,2016,16(6):348-353.
[17] HJ 656-2013,环境空气颗粒物(PM2. 5)手工监测方法(重量法)技术规范[S].
[18]贾佳,韩力慧,程水源,等.京津冀区域PM2. 5及二次无机组分污染特征研究[J].中国环境科学,2018,38(3):801-811.Jia J,Han L H,Cheng S Y,et al. Pollution characteristic of PM2. 5and secondary inorganic ions in Beijing-Tianjin-Hebei region[J]. China Environmental Science,2018,38(3):801-811.
[19]李凤菊,邵龙义,杨书申,等.郑州大气PM10的形貌特征及生物活性研究[J].环境科学,2008,29(9):2654-2658.Li F J,Shao L Y,Yang S S,et al. Morphology and bioreactivity of PM10in air of Zhengzhou[J]. Environmental Science,2008,29(9):2654-2658.
[20]郭家瑜,张英杰,郑海涛,等.北京2015年大气细颗粒物的空间分布特征及变化规律[J].环境科学学报,2017,37(7):2409-2419.Guo J Y,Zhang Y J,Zheng H T,et al. Characteristics of spatial distribution and variations of atmospheric fine particles in Beijing in 2015[J]. Acta Scientiae Circumstantiae,2017,37(7):2409-2419.
[21]吕佳莉,李萌,解静芳,等.太原城区PM2. 5重金属元素季节变化及形态分析[J].环境科学与技术,2016,39(4):126-131.Lyu J L,Li M,Xie J F,et al. Seasonal variation and chemical speciation analysis of heavy metal pollution in PM2. 5from urban area of Taiyuan[J]. Environmental Science&Technology,2016,39(4):126-131.
[22]王佳,李晓,吴瑞杰,等.郑州市PM2. 5和PM10中水溶性无机离子的污染特征[J].郑州大学学报(理学版),2014,46(4):81-87.Wang J,Li X,Wu R J,et al. Pollution characteristics of watersoluble ions in PM2. 5and PM10in Zhengzhou[J]. Journal of Zhengzhou University(Natural Science Edition),2014,46(4):81-87.
[23] Wang H L,Qiao L P,Lou S R,et al. Chemical composition of PM2. 5and meteorological impact among three years in urban Shanghai,China[J]. Journal of Cleaner Production,2016,112:1302-1311.
[24]吴耕晨.广州大气气溶胶水溶性组分分布特征的研究[D].广州:暨南大学,2015.Wu G C. Analysis of distribution characteristics for water soluble content in aerosol in Guangzhou[D]. Guangzhou:Jinan University,2015.
[25] Xu L L,Chen X Q,Chen J S,et al. Seasonal variations and chemical compositions of PM2. 5aerosol in the urban area of Fuzhou,China[J]. Atmospheric Research,2012,104-105:264-272.
[26]冯加良,胡小玲,管晶晶,等.上海市大气细颗粒物的酸度及其与组成的关系[J].上海大学学报(自然科学版),2010,16(5):431-436.Feng J L,Hu X L,Guan J J,et al. Acidity of PM2. 5in Shanghai and its correlation with chemical composition of the particles[J].Journal of Shanghai University(Natural Science),2010,16(5):431-436.
[27] Shon Z H,Ghosh S,Kim K H,et al. Analysis of water-soluble ions and their precursor gases over diurnal cycle[J].Atmospheric Research,2013,132-133:309-321.
[28] Han Y M,Du P X,Cao J J,et al. Multivariate analysis of heavy metal contamination in urban dusts of Xi'an,Central China[J].Science of the Total Environment,2006,355(1-3):176-186.
© 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 |